With the giant magnetoresistance (GMR) effect serving as a vital component in modern spintronic technologies, researchers are dedicating significant efforts to improve the performance of GMR devices through material exploration and design optimization. However, traditional GMR measurement approaches are inefficient for comprehensive material and device optimization. This study proposes a high‐throughput current‐in‐plane GMR measurement technique based on thermal imaging of Joule heating utilizing lock‐in thermography (LIT). This LIT‐based technique is advantageous for efficiently evaluating films with varying compositions and thickness gradients, which is crucial for ongoing material exploration and design optimization to enhance the GMR ratio. First, it is demonstrated that using CoFe/Cu multilayers, the simple Joule heating measurement based on LIT enables quantitative estimation of the GMR ratio. Then, to confirm the usefulness of the proposed method in high‐throughput material screening, a case study is shown to investigate the GMR of CoCu‐based granular films with a composition gradient. These techniques allow to determine the optimum composition with maximum GMR ratio using the single composition‐gradient film and reveal Co22Cu78 as the optimal composition, yielding the largest GMR ratio among the reported polycrystalline CoCu‐based granular films. This demonstration accelerates the material and structural optimization of GMR devices.