Materials that exhibit obvious pressure responses upon compression, such as hardening, compressibility and optical properties change, and so on, which have been explored as an important way to design new functional materials with desired mechanical properties and luminescent properties. Here, we will introduce some recent progress on the research of new pressure responsive functional crystalline materials with novel properties. A new strategy has been developed to design and construct new functional materials by application of high pressure to the designed co-crystals. The co-crystals have been designed based on carbon and carbon-based molecules and studied by high pressure technique. A series of new materials with potentially superhard properties, negative volume compressibility and anomalous pressure response in luminescence has been obtained.