Photonic crystal (PC) materials have huge potentials as sensors for noninvasive and real-time monitoring glucose in tears. We developed a glucose-sensitive PC material based on monolayered colloidal crystals (MCCs). Polystyrene nanoparticles were first self-assembled into a highly ordered MCC, and this two-dimensional (2D) template was then coated by a 4-boronobenzaldehyde-functionalized poly(vinyl alcohol) hydrogel. Such a sensor efficiently diffracts visible light, whose structural color could change from red through yellow to green, as the glucose concentration altered from 0 to 20 mM, covering both tears' and bloods' physiological ranges. The sensor also represents a rapid response within 180 s at each titration of glucose, combining the characteristics of high accuracy and sensitivity in detecting the glucose concentration in tears, and this intelligent sensing material presents certain possibility for the frontier point-of-care glucose monitoring.