Recently, we have developed a simple and green approach to surface wrinkling via lignification mimetic reaction and drying. A skin layer is synthesized on a chitosan film via immersion in a methanol solution containing a phenolic acid and subsequent surface reaction by horseradish peroxidase, mimicking wood lignification. A surface relief with micron-scale wrinkles is formed upon drying and as a result of inhomogeneous shrinkage. This focus review overviews this innovative approach and its detailed mechanism.