Human-serum-albumin (HSA)-templated molecularly imprinted polymer nanoparticles (nano-MIPs) were integrated with a solution-gated field-effect transistor-based biosensor. The real-time electrical analysis of nano-MIP-HSA binding showed a high affinity and specificity of nano-MIPs for HSA. Moreover, the binding behaviour was continuously visualised using a solution-gated complementary metal-oxide semiconductor array image biosensor.