Pulsed-laser deposition is a straightforward, versatile, and effective technique to form thin films of hard and soft materials on different substrates. This book presents an overview of how pulsed-laser deposition is used to form functional thin-film semiconductors on flexible plastic, glass, and gallium arsenide substrates. It gives insight into the characterizations of the photosensitive films. An interesting phenomenon, CdS / glass photocurrent quenching employing additional blue light excitation, is presented. The experimental results obtained in the photocurrent spectra measurement of CdS / plastic, CdS / glass, and ZnTe / GaAs hetero-paired employing pulsed-laser deposition are discussed in detail.