Combinatorial pulsed laser deposition (CPLD) using two targets was used to produce a range of transition metal-substituted perovskite-structured Sr(Ti(1-x)M(x))O(3-δ) films on buffered silicon substrates, where M = Fe, Cr, Ni and Mn and x = 0.05-0.5. CPLD produced samples whose composition vs distance fitted a linear combination of the compositions of the two targets. Sr(Ti(1-x)Fe(x))O(3-δ) films produced from a pair of perovskite targets (SrTiO(3) and SrFeO(3) or SrTiO(3) and SrTi0(0.575)Fe(0.425)O(3)) had properties similar to those of films produced from single targets, showing a single phase microstructure, a saturation magnetization of 0.5 μ(B)/Fe, and a strong out-of-plane magnetoelastic anisotropy at room temperature. Films produced from an SrTiO(3) and a metal oxide target consisted of majority perovskite phases with additional metal oxide (or metal in the case of Ni) phases. Films made from SrTiO(3) and Fe(2)O(3) targets retained the high magnetic anisotropy of Sr(Ti(1-x)Fe(x))O(3-δ), but had a much higher saturation magnetization than single-target films, reaching for example an out-of-plane coercivity of >2 kOe and a saturation magnetization of 125 emu/cm(3) at 24%Fe. This was attributed to the presence of maghemite or magnetite exchange-coupled to the Sr(Ti(1-x)Fe(x))O(3-δ). Films of Sr(Ti(1-x)Cr(x))O(3-δ) and Sr(Ti(1-x)Mn(x))O(3-δ) showed no room temperature ferromagnetism, but Sr(Ti(1-x)Ni(x))O(3-δ) did show a high anisotropy and magnetization attributed mainly to the perovskite phase. Combinatorial synthesis is shown to be an efficient process for enabling evaluation of the properties of epitaxial substituted perovskite films as well as multiphase films which have potential for a wide range of electronic, magnetic, optical, and catalytic applications.