A new method utilizing subsequent depositions of thin crack-free nanoparticle layers is demonstrated to avoid the formation of cracks within silica nanoparticle films. Using this method, films can be assembled with thicknesses exceeding the critical cracking values. Explanation of this observed phenomenon is hypothesized to mainly arise from chemical bond formation between neighboring silica nanoparticles. Application of this method for fabricating crack-free functional structures is demonstrated by producing crack-free Bragg reflectors that exhibit structural color.