Lost circulation control remains a challenge in drilling operations. Self-healing gels, capable of self-healing in fractures and forming entire gel block, exhibit excellent resilience and erosion resistance, thus finding extensive studies in lost circulation control. In this study, layered double hydroxide, Acrylic acid, 2-Acrylamido-2-methylpropane sulfonic acid, and CaCl2 were employed to synthesize organic-inorganic nanocomposite gel with self-healing properties. The chemical properties of nanocomposite gels were characterized using X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscope, X-ray photoelectron spectroscopy and thermogravimetric analysis. layered double hydroxide could be dispersed and exfoliated in the mixed solution of Acrylic acid and 2-Acrylamido-2-methylpropane sulfonic acid, and the swelling behavior, self-healing time, rheological properties, and mechanical performance of the nanocomposite gels were influenced by the addition of layered double hydroxide and Ca2+. Optimized nanocomposite gel AC6L3, at 90 °C, exhibits only a self-healing time of 3.5 h in bentonite mud, with a storage modulus of 4176 Pa, tensile strength of 6.02 kPa, and adhesive strength of 1.94 kPa. In comparison to conventional gel, the nanocomposite gel with self-healing capabilities demonstrated superior pressure-bearing capacity. Based on these characteristics, the nanocomposite gel proposed in this work hold promise as a candidate lost circulation material.