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In this article, we demonstrate a novel design of liquid crystal (LC) displays via predesigned radially constructed polydopamine (PDA) particles. The synthesized PDA particles were modified with dimethyloctadecyl-3-(trimethoxysilyl) propyl ammonium chloride (DMOAP) showing radial constructions. Both PDA particles and surface-modified PDA particles were used to disturb the order of the LC arrangement, showing an opaque appearance. Based on the results, the radially constructed PDA particles efficiently enhanced the performance of cholesteric liquid crystal (CLC) devices. Adding 0.1 wt% DMOAPmodified PDA particles into the CLC device shows a higher contrast of 82.2%, a lower threshold voltage of 2.4 V and a fast response time of 7.7 ms. Without adding polymer beads, no any display contrast was observed. The results suggest that the synthesized surface-modified PDA particles disturb the alignment of LCs dispersed in LC cells, leading to a great improvement in the contrast of the CLC devices. In addition, a prepared traditional polymer stabilized CLC (PSCLC) cell shows only 2.8% contrast. The best performance, with a high contrast of 93.8%, a low threshold voltage of 10.4 V and a fast response time of 10.2 ms, was achieved by adding 0.1 wt% modified PDA particles into the CLC device.