Eco-friendly clay-based adsorbents with low cost and high adsorption capacity for toxic dyes have attracted significant attention. In this study, a novel citric acid-modified sepiolite (CA-SEP) composite was developed for the efficient removal of methylene blue (MB) from aqueous solutions. The morphological, crystalline, and structural properties of the composite were characterized using XRD, FTIR, SEM, and BET analyses. Compared to pristine SEP, CA-SEP exhibited a 2.6-fold increase in adsorption capacity for MB and demonstrated excellent reusability. The effects of key parameters—including solution pH (2.0–10.0), contact time (0–300 min), adsorbent dosage (0.2–2.0 g/L), and initial MB concentration (10–150 mg/L)—on adsorption performance were systematically investigated. Modeling results indicated that the Sips isotherm provided the optimal fit for the equilibrium data. In kinetic studies, the adsorption process was best described by the pseudo-second-order model. The maximum adsorption capacity of CA-SEP for MB was estimated to be 40.61 mg/g. Moreover, the adsorbent retained high removal efficiency after five adsorption-desorption cycles, demonstrating good regenerability. These results indicate that CA-SEP is a highly efficient, sustainable, and economically viable adsorbent for the elimination of MB from contaminated water.