Microtruss cellular materials have large internal surface areas and small cross-sectional strut dimensions, permitting surface modification to substantially enhance their mechanical performance. For instance, a ~400% increase in compressive strength with virtually no weight penalty can be induced by a hard anodized Al₂O₃ ceramic coating of only ~50 µm thickness. The present study seeks the optimal architecture of these composites by exploring three research challenges:​ architecture and degree of forming are interdependent due to stretch-forming, architecture and the material properties are interdependent due to work-hardening, and ceramic structural coatings add design complexity. Theoretical predictions and architectural optimizations demonstrated a potential weight reduction of ~3% to ~60% through the increase of internal truss angle for both annealed and work-hardened microtruss cores. While further validation is needed, experimental evidence in this study suggested the collapse in ceramic-aluminum microtruss composites could be considered as a mixture of composite strut global buckling and oxide local shell buckling mechanisms.