Advances in zeolites research emerging from interdisciplinary efforts have opened new opportunities beyond conventional applications. Colloids drive much current research owing to their distinct collective behaviors, but so far, using zeolites as a colloidal building block to construct ordered superstructures remains unexplored. Herein we show that self-assembly of colloidal zeolite LTA superball (ZAS) by tilted-angle sedimentation forms macroscopic films with micro-mesoporosity and 3D long-range periodicity featuring a photonic band gap (PBG) that is tunable through the superball geometry and responds reversibly to chemical vapors. Remarkably, self-assembly of ZAS at elevated temperature forms 3D chiral photonic crystals that enable negative circular dichroism, selective reflection of right-handed circularly polarized (CP) light and left-handed CP luminescence based on PBG. We present a novel class of functional colloids and zeolite-based photonic crystals with the ability to manipulate light in several ways.