Composite based Ca/Al layered double hydroxide and biochar was prepared using mixing coprecipitation method at pH 10. Composite and the starting materials was characterized using X-ray, FTIR, BET, thermal, and SEM-EDX analyses. Furthermore, composite was used as adsorbent of methylene blue from aqueous solution. Several factors that influencing the adsorption process was investigated such as adsorption time, initial concentration, and temperature adsorption. The performance of composite as adsorbent was evaluated by reusability process. The results showed that composite has diffraction peak at 9.82, 17.99, 19.86, 20.55, 29.32, 30.95, 32.65, 36.61, 37.00, 43.49, 47.15, 55.12, and 56.12 deg, which was based on diffraction of Ca/Al layered double hydroxide and biochar as starting materials. The surface area of composite was 158.291 m2/g and largely higher than starting materials. The morphology of composite also shows regularity shape than Ca/Al layered double hydroxide and biochar. Adsorption of methylene blue on composite showed that higher adsorption capacity (32.535 mg/g) than starting materials. The reusability of adsorbent showed that composite can be used several times ad adsorbent without loss adsorption capacity and these phenomena indicated composite is excellent material to remove dye from aqueous solution.