This talk presents the combination of “bottom-up” layer-by-layer (LbL) nano self-assembly and “top-down” micromanufacturing techniques to fabricate MEMS and flexible electronics for biomedical applications. With nano self-assembly and surface micromachining, highly flexible nanoparticle-based cantilever platform for micro sensing and actuation was investigated successfully. With respect to flexible electronics, self-assembled graphene- and carbon nanotube-based field-effect transistors with embedded self-assembled films as dielectric and active layers were fabricated and characterized successfully. These self-assembled field-effect transistors were primarily investigated for high-performance bio-sensing applications.