 highlights uniaxial orientation and single-grain penetration of quasi-2D and 3D parafskite films were achieved via a general thermal-pressed TP strategy. The TP parafskite-based self-powered photodetectors, SPPDs, exhibit one of the best results among the 3D and quasi-2D parafskite SPPDs, respectively. These unpackaged TP-based devices exhibit ultra-high humidity, optical and heat stability. This article was authored by Faizhu, Ganglion, Delion Chouay, and others.