In this talk, I will describe the combinatorial materials research methodology we have developed using thin film techniques targeting a variety of functional materials. The basic idea of combinatorial thin film deposition systems is to create controlled compositional variation across given chips. Versatile compact combinatorial pulsed laser deposition systems are used for pursuing metal oxide systems. For studying metallic alloys, an UHV co-sputtering system is used to fabricate natural composition spreads. In this system, three magnetron guns are placed in a parallel geometry in order to maximize the coverage of ternary compositional phase space on three inch wafers. The spreads are primarily used for rapidly exploring novel phase space of magnetic materials. Various high-throughput characterization tools are used for rapid characterization of thin film combinatorial libraries and composition spreads. They include quantitative scanning microwave microscopes for studying dielectric/ferroelectric and resistive materials, scanning SQUID microscopes for mapping of magnetic properties and a scanning X-ray diffractometer for structural characterization. We also implement micromachined device libraries such as arrays of cantilevers for investigation of smart materials. Our studies have led to identification of novel compositional regions of ferromagnetic shape memory alloys.