AbstractPulsed laser micropropulsion (PLMP) offers a promising avenue for miniature space craft, yet conventional propellants face challenges in balancing efficiency and stability. An optical‐propulsion metastructure strategy using metal‐organic frameworks (MOFs) is presented to generate graphene‐metal metastructures (GMM), specifically GMM‐(HKUST‐1), which significantly enhances PLMP performance. This novel approach leverages the unique interaction between pulsed lasers and the precisely engineered GMMs—comprising optimized metal nanoparticle size, graphene layers, and inter‐particle gaps—to boost both propulsion efficiency and stability. Experimental and numerical analyses reveal that GMM‐(HKUST‐1) achieves aspecific impulse of 1072.94 s, ablation efficiency of 51.22%, and impulse thrust per mass of 105.15 µN µg−1, surpassing traditional propellants. With an average particle size of ≈12 nm and a density of 0.958 g cm−3, these metastructures exhibit 99% light absorption efficiency and maintain stability under atmospheric and humid conditions. The graphene nanolayer efficiently absorbs and converts laser energy, while the metal nanostructures enhance light‐matter interactions, promoting energy transfer and material stability. These findings suggest that this GMM‐based optical‐propulsion strategy can revolutionize microspacecraft propulsion and energy systems, offering significant advancements across various domains.