Without doubt, one of the most fascinating questions ever asked is “What is life?”, immediately followed by “How and where did life arise?”. Both questions are by no means exclusively related to chemistry and biology. Indeed, it was soon realized that concepts from astrophysics, geochemistry, geophysics, planetology, earth science, bioinformatics, complexity theory, mathematics and many more are needed to figure out sensible answers. This themed issue focuses on a specific and very intriguing aspect of the problem, i.e. the evolutionary chemical steps that brought simple molecules towards a kind of self-organization, which ultimately gave rise to the first biopolymers and to proto-metabolism. This is a key point as today life is sustained by the intricate biochemistry occurring within extremely complex cells, which were obviously absent in the early days of prebiotic chemistry. Astrochemical evolution has been able to give rise only to very simple inorganic compounds according to current knowledge. Research on how life emerged on our primitive Earth from very simple inorganic compounds started in the 1950s with the famous Miller experiment and involves an interdisciplinary approach, which is well represented in this issue, and is by no means limited to chemistry, in complete agreement with D. Deamer's statement from his book “First Life” that “life can emerge where physics and chemistry intersect”. The search for life's signature on other worlds, at least in our solar system, is described in three contributions, all devoted to clarifying the fascinating chemistry happening on Titan, the largest moon of Saturn. Raulin and co-workers (DOI: 10.1039/C2CS35014A) merge observations from the Cassini–Huygens mission with theoretical modeling and experimental simulations to provide a detailed view of the complexity of Titan's atmosphere, which is relevant as a model of the primitive upper terrestrial atmosphere. Kaiser and Mebel (DOI: 10.1039/C2CS35068H) combine an experimental approach (crossed molecular beams reactions) with sophisticated quantum mechanical methods to describe the complex reaction pathways leading to the formation of polyacetylenes and cyanopolyacetylenes in Titan's aerosol layers. Balucani (DOI: 10.1039/C2CS35113G) uses the same combination of experimental and theoretical techniques to disentangle the intricate elementary reactions involving N atoms and hydrocarbons to bring about prebiotic N-containing molecules in Titan's planetary atmosphere. The contributions from Meierhenrich and Burton both focus on the way in which the chirality of amino acids and nucleobases, which is an essential feature of today's biomolecules, was developed. Meierhenrich and co-workers (DOI: 10.1039/C2CS35051C) review simulated experiments mimicking the harsh conditions of the interstellar medium as well as the exciting Rosetta mission expected to land on the 67P/Churyumov–Gerasimenko comet in 2014. The review of Burton and co-workers (DOI: 10.1039/C2CS35109A) specifically focuses on carbonaceous chondrite meteorites and the subtle analytical techniques allowing to evidence the wide range of organic compounds, including amino acids and nucleobases, that may have been delivered to the early Earth through meteoritic bombardment, contributing to the origin of life. Prebiotic chemical formation of N-containing heterocycles is the topic of the contribution by Menor-Salván and Marín-Yaseli (DOI: 10.1039/C2CS35060B) who studied experimentally the fascinating chemistry occurring at the ice–liquid water interface. This chemistry provides clues about the origin of nucleobases in the inner solar system bodies. A different kind of interface is addressed in the work by Cleaves and co-workers (DOI: 10.1039/C2CS35112A) who first defined the pool of possible minerals present on planet Earth before 3.5 Gy and then focused on the mineral–organic interface as a key step in many important aspects of prebiotic chemistry due to the thermodynamic and catalytic effects of mineral surfaces, which may have played an essential role in bringing simple molecules to the complexity level of proto-biopolymers. The feasible chemical pathways and physico-chemical requirements for bringing simple amino acids to evolve into peptides, including stereoselectivity, are addressed in depth by Pascal and co-workers (DOI: 10.1039/C2CS35064E). The work by Jakschitz and Rode (DOI: 10.1039/C2CS35073D) provides a unifying version of the condensation of amino acids to peptides and the development of their homochirality based on the salt induced peptide formation reaction. Coveney and co-workers (DOI: 10.1039/C2CS35018A) use simulation and modeling tools to understand chiral amplification and vesicle formation kinetics, as well as quantum mechanics to understand the atomistic details of reactions occurring at the mineral surface. The key questions concerning complex chemical auto-organization leading to metabolic networks are addressed by Peretó (DOI: 10.1039/C2CS35054H), whereas Di Mauro, Saladino and co-workers (DOI: 10.1039/C2CS35066A) tackle the old “chicken-or-egg” question of which process, genetics or metabolism, came first at the origin of life. This question might be overcome if formamide is adopted as a prebiotic molecule, because its chemistry may unify metabolism and genetics. Present day cells are enormously complicated bags of exquisitely organised biomolecules and this complexity was not present originally. However, it has long been recognised that compartmentalisation is essential for life to evolve. The contribution by Deamer (DOI: 10.1039/C2CS35042D) shows how liquid crystalline nanostructures are crucial for catalysing non-enzymatic nucleic acid polymerisation by means of hydration/dehydration cycles, which provide the needed activation energy. Some breakthroughs have already been achieved while trying to answer the big questions asked at the beginning of this introduction, as testified by the number of excellent reviews in this themed issue, yet a lot of work remains to be done. We are deeply convinced that beyond the borders of the traditional domains of scientific activity, the multidisciplinary character of the present topic leaves room for anyone trying to creatively contribute to the improvement of our understanding of the origin of life on rigorous scientific grounds. We have been honored to help in gathering the contributions to this issue from many distinguished experts of the field and we hope this work will be stimulating to many young scientists.