asymmetric chemical properties, both in bulk and in surface-confined coatings. [1][2][3][4][5] Referencing their two-faced nature, such asymmetric material properties are often named after the Roman god Janus. In particular, the behavior of membranes, particles, rods, or micelles with two orthogonal sides shows high potential for different applications, such as oil/water separation, droplet manipulation, fog collection, unidirectional water flow design, bubble aeration, ion gating, and energy harvesting. [6][7][8][9][10][11][12] In particular, asymmetrically designed membranes show strong potential for improved transport design and thus improved application performance. Directed oil-water transport in the context of oil-water separation and directed gas-water transport in the context of fuel cell gas diffusion layers are two specific application examples. [13,14] Therefore, enhancing control of material design and reducing the amount of material needed to achieve asymmetric material characteristics such as wettability are still an ongoing challenge. To make this situation even more stimulating, applying biocompatible and degradable materials while retaining needed stability and doing this in simple, ideally single-step, scalable fabrication processes are of increasing demand.Janus materials in general are well known since the Nobel Prize lecture of de Gennes in 1991, but they were first mentioned in 1898 by the group of Veyssié. [15,16] The general definition of Janus materials is diverse and includes all materials with asymmetric surfaces as well as composite bulk materials. In 2016, the group of Xu reshaped the definition of materials having opposing properties at two respective interfaces and proposed three configurations of so-called Janus membranes. [5] One is the "A to B"-type material, which shows a physical and/or chemical gradient across a membrane cross-section. Alternatively, A-to-B or A-and B-type Janus membranes are defined as having a clear interface between the layers. Within the last few years, the Jiang group developed a coating and peeling strategy for the facile preparation of multifunctional Janus membranes based on synthetic polymers such as polyethylene terephthalate (PET)/polytetrafluoroethylene (PTFE). [1] After membrane modification by tannic acid (TA) and diethylenetriamine to form a hydrophilic coating on the surface, peeling off the top PTFE layer from the hydrophilic membrane results in a Janus membrane showing unidirectional water permeation properties at Functional paper-based materials and devices have been increasingly attractive to scientists in the recent past. In particular, the possibility to functionalize the surface of paper fibers with tailor-made coatings has broadened a possible scope of emerging application considerably. This work introduces novel functional paper membranes with adjustable gradient and Janus-type wettability based on gradient and Janus-type silica coating distribution along the paper cross-section. Correlation of CLSM (distribution), thermogravimetric an...