A method for plugging and sealing subsurface formations using alkaline nanosilica dispersion and a delayed activation chemistry is disclosed. In accordance with one embodiment of the present disclosure, the method includes introducing a mixture with a first pH into the subsurface formation. The mixture comprises an aqueous solution, an alkaline nanosilica dispersion and a water-insoluble hydrolyzable compound. The method further includes allowing the water-insoluble hydrolyzable compound to hydrolyze in the subsurface formation to form an acid at 70° C. or greater, thereby acidizing the mixture to a reduced second pH and causing the alkaline nanosilica dispersion to gel into a solid and seal the subsurface formation. A composition for sealing a subsurface formation is also disclosed. The composition includes an aqueous mixture including water, an alkaline nanosilica dispersion, and a water-insoluble hydrolyzable compound.