Lipid droplets (LDs), hubs of neutral lipid storage and distribution, have been shown in cryoEM to undergo a liquid-crystalline phase transition under high sterol ester (SE) concentrations, forming concentric rings like layers of an onion. This research sought to characterize this phase transformation at the molecular level. After developing sterol ester parameters, we were able to capture this phase transformation with 90% SE in 3 microseconds of simulation. Interestingly, the ordered layers of SEs in the LD core transformed the phospholipid monolayer surrounding the LD as well: increasing lipid packing and tail order parameters, while squeezing out surface neutral lipids and significantly diminishing membrane packing defects. We discuss how these changes will have profound effects on LD-protein interactions, consistent with experimentally demonstrated altered LD proteomes.