The propagation control of chemical waves via a pentagonal patterned structure in a self‐oscillating polymer brush composed of N‐isopropylacrylamide and a metal catalyst for the Belousov–Zhabotinsky (BZ) reaction is reported. The patterned self‐oscillating polymer brush is prepared by combining surface‐initiated atom transfer radical polymerization and maskless photolithography. Surface modification is confirmed by X‐ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, 3D measuring laser microscopy, and fluorescence microscopy. The polymer brush patterns are fabricated with gaps between the pentagonal regions, and investigations on the effect of the gap distance on the BZ reaction reveal that at the appropriate distance, chemical waves propagate across the array from the plane to the corner between the patterns. Unidirectional control is achieved not only in the 1D array, but also in a 2D curved array. This patterned self‐oscillating polymer brush is a novel and advantageous approach for creating an autonomous dynamic soft interface.