We have developed a sequential process for the fabrication of enhanced‐grain thin‐film CuInSe2‐based photovoltaic devices. In this process, exact control of the composition during fabrication is not necessary. Analysis of the film structures suggests enhanced grain size, transport, and photoconductivity. Device structures vary from one‐sided heterojunctions to buried homojunctions where the window layer is not required for photo‐response. We have also developed a fabrication process that incorporates variable elemental fluxes and flux ratios, and a substrate temperature of 550 °C. Preliminary results include a fill‐factor of 75%, a diode factor of 1.2, and enhanced spectral response in the near‐infrared region. We present an update on this work and attempt to describe the relationship between the growth dynamics and the resultant material and device performance. The results suggest new approaches to the fabrication of high efficiency CuInSe2‐based solar cells.