Liposomes coated with chitosan by ionic gelation with tripolyphosphate (TPP-chitosomes) are interesting particles for stabilizing active compounds. However, the encapsulation condition must be optimized. The aim of this study was to optimize the encapsulation of phenolics and carotenoids of carrot pomace in TPP-chitosomes by using a Central Composite Design 2 and response surface methodology. The independent variables were the phospholipid (0.8-4.2 mg/mL), chitosan (2.6-9.4 mg/mL), and carrot pomace (4-14 g/100 mL of ethanol) concentrations; the responses were the encapsulation efficiency in TPP-chitosomes (EE) of phenolics, a-carotene, and b-carotene and the particle size and zeta potential of the particles. The zeta potential ranged from +17 to +37 mV, indicating that the liposomes were coated with chitosan and that the particle sizes were in the nanometric to submicrometric scale. The optimized condition for encapsulating carotenoids was 2.5 mg/mL phospholipids, 6.0 mg/mL chitosan, and 12 g of carrot pomace/100 mL of ethanol. In this condition, the EE of phenolics and α- and β-carotene was 95%, 98%, and 99%, respectively. Therefore, TPP-chitosomes containing encapsulated phenolics and carotenoids, which can be obtained from agro-industrial by-products, have potential application as natural pigments in food or cosmetics. TPP-chitosomes can also be used to encapsulate other types of natural pigments.