Polymer-based porous hybrid materials (PHMs) carrying inorganic c on the surface of pores have important applications in chemical and biological sensing, in chromatography, and in heterogeneous catalysis. This Feature Article provides an overview of the recent developments in the synthesis and fabrication of multifunctional PHMs using polymerization-induced phase separation. Exemplary applications of a PHM coated with gold nanorods were demonstrated for the simultaneous detection of different analytes using surface enhanced Raman scattering (SERS) spectroscopy and fluorescence microscopy.