3D optical crystals have found their applications in sensing, actuation, optical devices, batteries, supercapacitors, etc. The 3D optical crystal devices are comprised of two main components: colloidal gels and nanoparticles. Nanoparticles self-assemble into face center cubic structures in colloidal gels. The inherent 3D optical crystal structure leads to display of structural colors on these devices following light impingement. As such, these optical properties have led to the utilization of these 3D optical crystals as self-reporting colorimetric sensors, which is the focus of this review paper. While there is extensive work done so far on these materials to exhaustively be covered in this review, we focus here in on: mechanism of color display, materials and preparation of 3D optical crystals, introduction of recent sensing examples, and combination of 3D optical crystals with molecular imprinting technology. The aim of this review is to familiarize the reader with recent developments in the area and to encourage further research in this field to overcome some of its challenges as well as to inspire creative innovations of these materials.