Ink-based semiconductors that come to mind today include conjugated molecules and polymers, colloidal quantum dots, metal halide hybrid perovskites, and transition metal oxides. These materials form an ink (solution/ suspension/ sol-gel) that can be applied and dried in ambient air to form high-quality films for optoelectronic devices. In this study, we will introduce the current understanding of ink-based lead and lead-free hybrid perovskite and perovskite-inspired thin films. Examples will be presented through time-resolved studies of the solidification to link the solid-state microstructure and device figures of merit to the ink’s formulation, drying, and solidification process. The perovskite crystallization kinetics characterized in situ during the solution process indicates an essential role by the inclusion of Cs+ and K+ alkali metal cations in perovskite inks. The film and device characterizations indicate the functions of mixed cation and halides in determining the optoelectronic properties. The further sophisticated design of perovskite inks enables significantly optimized charge dynamics, including exciton separation, inter-grain charge transfer, trap density, charge mobility, and charge collection efficiency. The considerably improved optoelectronic properties lead to higher charge collection efficiency and, therefore, better open-circuit voltage and fill factor for the Cs+-containing 3D perovskite devices in contrast to the control FAPbI3 one. Recent developments in ink formulation and processing that enable scalable ambient fabrication of high-quality perovskite semiconductor films will also be presented. These findings raise the possibility of developing more controlled perovskites for systematically addressing both charge dynamics and degradation mechanisms in concert for the timely commercialization of perovskite solar cells.