We present here our results on using liquid crystals (LCs) in experiments with nonclassical light sources: (1) single-photon sources exhibiting antibunching (separation of all photons in time), which are key components for secure quantum communication systems and (2) entangled photon source with photons exhibiting quantum interference in a Hong–Ou–Mandel interferometer. In the first part, both nematic and cholesteric liquid crystal (CLC) hosts were used to create definite linear or circular polarization of antibunched photons emitted by different types of single emitters (dye molecules, nanocrystal quantum dots (NQDs), nanodiamonds with color centers, etc.). If the photon has unknown polarization, filtering it through a polarizer to produce the desired polarization for quantum key distribution with bits based on polarization states of photons will reduce by half the efficiency of a quantum cryptography system. In the first part, we also provide our results on observation of a circular polarized microcavity resonance in NQD fluorescence in a 1-D chiral photonic bandgap CLC microcavity. In the second part of this paper with indistinguishable, time-entangled photons, we demonstrate our experimental results on simulating quantum mechanical barrier tunneling phenomena. A Hong–Ou–Mandel dip (quantum interference effect) is shifted when a phase change was introduced on the way of one of entangled photons in pair (one arm of the interferometer) by inserting in this arm an electrically controlled planar-aligned nematic LC layer between two prisms in the conditions close to a frustrated total internal reflection. By applying different AC-voltages to the planar-aligned nematic layer and changing its refractive index, we can obtain various conditions for incident photon propagation – from total reflection to total transmission. Measuring changes of tunneling times of photon through this structure with femtosecond resolution permitted us to answer some unresolved questions in quantum mechanical barrier tunneling phenomena.