We demonstrate the effective establishment of long-range electrostatic interactions among colloidal silica nanospheres through acid treatment, enabling their assembly into colloidal crystals at remarkably low concentrations. This novel method overcomes the conventional limitation in colloidal silica assembly by removing entrapped NH4+ ions and enhancing the electrical double layer (EDL) thickness, offering a time-efficient alternative to increase electrostatic interactions compared with methods like dialysis. The increased EDL thickness facilitates the assembly of SiO2 nanospheres into a body-centered-cubic lattice structure at low particle concentrations, allowing for broad spectrum tunability and high tolerance to particle size polydispersity. Further, we uncover a disorder-order transition during colloidal crystallization at low particle concentrations, with the optimal concentration for crystal formation governed by both thermodynamic and kinetic factors. This work not only provides insights into assembly mechanisms but also paves the way for the design and functionalization of colloidal silica-based photonic crystals in diverse applications.