We demonstrate nano-structural characteristics of carbon nanotube (CNT)-polydimethylsiloxane (PDMS) composite films that can be used as highly efficient and robust ultrasound transmitters for diagnostic and therapeutic applications. An inherent architecture of the nano-composite provides unique thermal, optical, and mechanical properties that are accommodated not just for efficient energy conversion but also for extraordinary robustness against pulsed laser ablation. First, we explain a thermoacoustic transfer mechanism within the nano-composite. CNT morphologies are examined to determine a suitable arrangement for heat transfer to the surrounding PDMS. Next, we introduce an approach to enhance optical extinction of the composite films, which uses shadowed deposition of a thin Au layer through an as-grown CNT network. Finally, the transmitter robustness is quantified in terms of laser-induced damage threshold. This reveals that the CNT-PDMS films can withstand an order-of-magnitude higher optical fluence (and extinction) than a Cr film used as a reference. Such robustness is crucial to increase the maximum-available optical energy for optoacoustic excitation and pressure generation. All of these structure-originated characteristics manifest the CNT-PDMS composite films as excellent optoacoustic transmitters for high-amplitude and high-frequency ultrasound generation.