On the basis of the self-catalytic characteristic of alpha-aminomethyl triethoxysilanes, (diethyl) aminomethyl triethoxysilane, cyclohexylaminomethyl triethoxysilane, and anilinomethyl triethoxysilane were used as self-catalytic cross-linkers to prepare a series of environmental friendly, nano-CaCO3 reinforced silicone sealants based on poly(dimethylsiloxane) (PDMS). The tensile properties, hardness, adhesive properties, hot-air aging resistance, and oil-resistance properties of these materials were studied by universal electronic tensile machine, scanning electron microscope, and atomic force microscopy, etc. Results show that the comprehensive properties of the self-catalytic cross-linking PDMS sealants are much better than that of the traditional ones. The chemical structure and reactivity of the a-aminomethyl triethoxysilanes have a great effect on the properties of PDMS sealants. The tensile strength of the reinforced sealants with 100 phr (100 parts per hundreds of PDMS) nano-CaCO3 is about 4.4 times than that of the unreinforced ones, and the elongation at break is about three times. POLYM. ENG. SCI., 51: 1033-1040, 2011. (C) 2011 Society of Plastics Engineers