Therapeutic artificial cells or organelles are nanoengineered vehicles that are expected to substitute for missing or lost cellular function. The creation of capsosomes, polymer carrier capsules containing liposomal subcompartments, is a promising approach towards constructing such therapeutic devices using the layer-by-layer assembly method. Herein, the assembly of intact, nonaggregated capsosomes containing multiple liposome layers is reported. It is also further demonstrated that thiocoraline, a hydrophobic model peptide with antitumor activity, can be efficiently loaded into the membrane of the liposomal subcompartments of the capsosomes. Cell viability assays verify the activity of the trapped antitumor cargo. It is also shown that pristine capsosomes do not display inherent cytotoxic effects. The ability to tune the number of liposome layers and hence the drug loading in capsosomes as well as their noncytotoxicity provide new opportunities for the creation of therapeutic artificial cells and organelles.