Fourier transform infrared (FTIR) spectroscopic imaging with infrared array detectors has recently emerged as a powerful materials characterization tool. We report a novel application of FTIR imaging for high-throughput analysis of materials under controlled environment. This approach combines the use of spectroscopic imaging with an attenuated total reflection (ATR)-IR cell, microdroplet sample deposition system, and a device that controls humidity inside the cell. By this approach, it was possible to obtain "chemical snapshots" from a spatially defined array of many different polymer/drug formulations (more than 100) under identical conditions. This method provides direct measurement of materials properties for high-throughput formulation design and optimization. Simultaneous response (water sorption, crystallization, etc.) of the array of formulations to the environmental parameters was studied. Implications of the presented approach range from studies of smart polymeric materials and sensors to screening of pharmaceuticals and biomaterials.