<p>In this study, a methodological framework was developed and validated for the analysis of crocin I (SI), crocin II (SII), and picrocrocin (SIII) in <i>Crocus sativus</i> L. residue (CSLR). This framework employed instrumental thin-layer chromatography (TLC) to ensure the reliability and precision of the analytical process. Instrumental TLC analysis was performed on a silica gel G F₂₅₄ plate with an ethyl acetate‒methanol‒water (6.5:2:2, <i>V/V</i>) mixture as the mobile phase. Qualitative and quantitative analysis were performed at a wavelength of 254&#xa0;nm. The linear ranges of SI, SII, and SIII in the instrumental TLC method were determined to be 0.30‒1.40, 0.20‒0.90, and 0.19‒0.85&#xa0;μg, respectively. The corresponding correlation coefficients (<i>R</i>²) were found to exceed 0.99, indicating a highly significant relationship between the observed and measured values. The precision, stability, and relative standard deviation of the instrumental TLC method were found to be less than 3.0%. The recovery values of SI, SII, and SIII measured using the instrumental TLC method were 101.4%, 99.5%, and 98.4%, respectively. This provides reliable methodological support for the quality evaluation of CSLR and subsequent research. The values of SI, SII, and SIII extracted from CSLR can be transformed to facilitate the reuse of resources and environmental protection.</p>