Nanotechnologies represent an unprecedented recent advance that may revolutionize many areas of medicine and biology, including cancer diagnostics and treatment. Nanoparticle-based technologies have demonstrated especially high potential for medical purposes, ranging from diagnosing diseases to providing novel therapies. However, to be clinically relevant, the existing nanoparticle-based technologies must overcome several challenges, including selective nanoparticle delivery, potential cytotoxicity, imaging of nanoparticles, and real-time assessment of their therapeutic efficacy. This review addresses these issues by summarizing the recent advances in medical diagnostics and therapy with a focus on the self-assembly of gold nanoparticles into nanoclusters in live cells, in combination with their detection using photothermal (PT) techniques.