Doped manganites, RE 1-x A x MnO 3 (RE = rare-earth and A= alkaline-earth elements), have attracted much attention because of their potential applications in magnetic sensors and other devices. [1][2][3][4][5] A prominent feature of these materials is a metallic-insulating (MI) transition associated with the ferromagnetic-paramagnetic (FM-PM) transition.[4] The figure of merit of these colossal magnetoresistance (CMR) materials for many applications is the magnetoresistance (MR = (q Hq 0 )/q 0 , where q H and q 0 are the resistivities with and without a magnetic field, respectively). For practical applications, it is important to obtain a high MR at room temperature and at low magnetic fields. It has been observed that the MR near or at the transition temperature, T c , for a given field strength, is generally larger for samples with lower T c .[2] Thus, simply changing the composition of these manganites is not effective in obtaining large MR values near room temperature. Many recent efforts in searching for enhanced MR have been focused on transport properties across artificial grain boundaries and interfaces by making FM manganite/spacer superlattices and FM-insulator-FM tunneling junctions. [6][7][8] However, the enhancements of the MR were mostly achieved at low temperatures (< 150 K). [5]In this work, we report our efforts to obtain a large MR near room temperature by preparing multilayer-coated La 0.67 Sr 0.33 MnO 3 /La 0.67 Ca 0.33 MnO 3 (LSMO/LCMO) films using polymer assisted deposition (PAD). PAD is a solution technique that has been successfully used to prepare both simple and complex metal oxide films. [11,12] The LSMO and LCMO compounds have similar lattice parameters and have a Curie temperature above and below room temperature, respectively, which makes them very attractive for preparing multilayers. The PAD technique was used to prepare the solutions of La 0.67 Sr 0.33 Mn and La 0.67 Ca 0.33 Mn. These solutions were spincoated onto single-crystalline (001) LaAlO 3 (LAO) substrates. After each coating, the films were heated at 600°C for 5 min. For all the films, a total of 10 coatings were applied on the substrate and final annealing was performed at 950°C for 2 h in oxygen. The thicknesses of the films were ca. 130 nm. Our initial study focused on optimizing the LSMO/LCMO ratio to get a maximum MR close to room temperature. The films with LSMO/LCMO volume ratios of 70:30, 60:40, and 50:50 had MR values of -61 %, -63 %, and -57 %, respectively, at 300 K at an applied field of 5 T. Hence, in this work we prepared multilayer-coated films by holding the LSMO/ LCMO volume ratio constant (60:40 with maximum MR) and changing the number and the thickness of the individual layers. Details of the layered configuration with their sample identifications (ML1 and ML2) are illustrated in Figure 1. To make a direct comparison of the multilayer-coated films, a single-phase film of La 0.67 Sr 0.198 Ca 0.132 MnO 3 (LSCMO), which is a uniformly mixed phase of the LSMO/LCMO at a volume ratio of 60:40, was also prepa...