The green development of stabilizers is an important part of soil health management. Studying the impact of stabilizers on soil cadmium (Cd) adsorption is critical for sustainable agriculture. Calcium-aluminum layered double hydroxides (Ca-Al-LDH) are widely used to detoxify contaminated water and soil. Nevertheless, little is known about the efficacy of Ca-Al-LDH at modulating the heavy metal bioavailability of various crops. Incubation experiments, greenhouse and 3-year field trials were conducted to investigate the effects of Ca-Al-LDH on Cd, lead (Pb), and zinc (Zn) bioavailability in different soil-crop systems. The main soil type was hydragric anthrosols. The results showed that Ca-Al-LDH remediate heavy metal pollution through surface complexation, surface precipitation, and metal cation exchange with alkali. In incubation experiments, the application of 3 % Ca-Al-LDH for 7–42 d significantly decreased soil CaCl₂-extractable Cd, Zn, and Pb by 94.38–96.37 %, 77.90–94.22 %, and 7.23–56.79 %, respectively, relative to the control (p < 0.05). It significantly lowered the exchangeable Cd fraction while increasing the carbonate-bound and the iron-manganese oxide-bound Cd fractions in the incubation and pot experiments. It significantly reduced the Cd content in bioaccumulator crops such as spinach, celery, amaranth, Shanghai bok choy, and lettuce-an. The Cd content in low-Cd-accumulation vegetables, such as bok choy, swamp cabbage, and lettuce-ra, increased following Ca-Al-LDH treatment to soil. Ca-Al-LDH activity remained stable for 3 years. The present study demonstrated that Ca-Al-LDH is a highly effective, sustainable, and versatile amendment for planting high-Cd vegetable cultivars. However, it should be avoided in areas with low Cd contamination or cautiously used when growing vegetables with low Cd-accumulation. It provides a theoretical and practical foundation for evaluating stabilizers and soil health management to remediate Cd-contaminated agricultural soils.