Centimeter-scale poly(acrylic acid-co-DVB80) (PAA) 3D colloidal crystal belts were prepared via a novel robust vertical deposition technique based on negative pressure and curvature substrate of the glass vial. The formation of PAA colloidal crystal belts was investigated. The results indicated that curvature could control the dimension of PAA colloidal crystal belts. Well-controlled negative pressure resulted in rapid fabrication of well-defined PAA colloidal crystal belts. Curvature substrate of glass vial could distribute shrinking stress in the process of drying of colloidal films. Strong hydrogen bonding interactions among carboxyl groups on the surface of PAA colloidal particles was responsible for PAA colloidal crystal belts with closed-packing characteristics.