The Last Level Cache (LLC) is the processor’s critical bridge between on-chip and off-chip memory levels - optimized for high density, high bandwidth, and low operation energy. To date, high-density (HD) SRAM has been the conventional device of choice; however, with the slowing of transistor scaling, as reflected in the industry’s almost identical HD SRAM cell size from 5 nm to 3 nm, alternative solutions such as 3D stacking with advanced packaging (i.e., hybrid bonding) are pursued (as demonstrated in AMD’s V-cache). Escalating data demands necessitate ultra-large on-chip caches to decrease costly off-chip memory movement, pushing the exploration of device technology towards monolithic 3D (M3D) integration, where transistors can be stacked in the back-end-of-line (BEOL) at the interconnect level. M3D integration requires fabrication techniques compatible with a low thermal budget (seconds) when used in a gain-cell configuration. This paper examines device, circuit, and system-level tradeoffs made when optimizing BEOL-compatible AOS-based 2-transistor gain cells (2T-GC) for LLC. A cache early-exploration tool, NS-Cache, is developed to model caches in advanced 7 & 3 nm nodes and is integrated with the Gem5 simulator to systematically benchmark the impact of the newfound density/performance when compared to HD-SRAM, MRAM, and 1T1C eDRAM alternatives for LLC.