The ability to monitor sub-micrometer gas vesicles' (GVs) vibration behavior to nonlinear buckling and collapse using laser Doppler vibrometry is reported, providing a precise noncontact technique for monitoring the motion of sub-micrometer objects. The fundamental and first harmonic resonance frequencies of the vesicles are found to be 1.024 and 1.710 GHz, respectively. An interparticle resonance is furthermore identified at ≈300 MHz, inversely dependent upon the agglomerated GV size of around 615 nm. Most importantly, the vesicles amplify and broaden input acoustic signals at far lower frequencies-for example, 7 MHz-associated with medical and industrial applications, and they are found to transition from a linear to nonlinear response at 150 kPa and to collapse at 350 kPa or greater.