Continuous　developments　of　innovative　anticounterfeiting　strategies　are　vital　to　restrain　the　fast-growing　counterfeit　markets.　Physical　unclonable　function　(PUF)-based　taggants　allow　for　a　practical　solution　to　provide　irreproducible　codes　for　strong　authentication.　Herein,　an　advanced　anticounterfeiting　strategy　with　multiple　security　levels　was　successfully　developed　using　screen　printing　and　atomic　layer　infiltration　(ALI)　techniques.　Macroscale　poly(dimethylsiloxane)　(PDMS)　patterns　were　fabricated　for　primary　verification.　Spontaneous　formation　of　random　wrinkles　with　size　in　the　micrometer　scale　was　achieved　on　the　top　surface　of　screen-printed　PDMS　patterns　due　to　the　anisotropic　relief　and　redistribution　of　extra　compressive　stress　after　Al2O3　infiltration,　which　can　be　used　for　senior　authentication　by　image　identification　using　the　artificial　intelligence　(AI)　technique.　Furthermore,　the　complexity　and　security　level　of　a　code,　which　are　proportional　to　the　minutia　density,　can　be　adjusted　by　the　morphology　of　the　wrinkles　in　terms　of　amplitude　and　wavelength　via　the　degree　of　Al2O3　permeation　depending　on　ALI　conditions.　These　spontaneously　formed　random　wrinkles　were　demonstrated　for　validation　and　decoding　with　AI,　exhibiting　the　merits　of　being　unclonable,　nondestructive,　universally　adaptable,　environmentally　stable,　and　mass-producible,　and　sufficiently　adaptable　for　an　industry-suitable　authentication　strategy.　©　2021　American　Chemical　Society.　All　rights　reserved.