Microbubbles offer unique properties as combined carriers of therapeutic payloads and diagnostic agents. Here we report on the development of novel microbubble architectures that in addition to the usual lipid shell have an actin cytoskeletal cortex assembled on their exterior. We show, using atomic force microscopy that this biomimetic coating creates a thin mesh that allows tuning of the mechanical properties of microbubbles and that the nature of actin assembly is determined by the fluidity of the lipid layer. Further, we show that it is possible to attach payloads and targeting-ligands to the actin scaffold. Resistance to gas permeation showed that the additional actin layer reduces gas diffusion across the shell and thus increases bubble lifetime. This study demonstrates a one step method to creating more complex microbubble architectures, which would be capable of further modification and tuning through the inclusion of actin binding proteins.