Harvesting the properties of nanosheets is not only crucial from af undamental perspective,b ut also for the development of novel functional devices based on 2D nanosheets.H erein, we demonstrate the processing of organically modified TBA x H 1Àx Ca 2 Nb 3 O 10 nanosheets into photonic thin films and study their colorimetric sensing properties in response to various aqueous and organic solvent vapors. Building on the enhanced solvent accessibility of TBAcontaining nanosheets and their photocatalytic activity under UV irradiation, we develop an ew concept for photocatalytic lithography using TBA x H 1Àx Ca 2 Nb 3 O 10 nanosheets as an egative photoresist to obtain high-fidelity micron-scale patterns of robust inorganic nanosheets.P hotocatalytic nanosheet lithography (PNL) therefore adds anew resist-free,resource efficient direct patterning technique to the toolbox of photolithography.Recently,calcium niobate nanosheets derived from the Dion-Jacobson-type perovskite HCa 2 Nb 3 O 10 have developed into an ubiquitous building block for nanoarchitectonics, [1] nanoelectronics, [2] and beyond [3] owing to their high structural definition and aspect ratio as well as their easy accessibility and handling. [2c, 4] Amongst others,c alcium niobate nanosheets have been deployed as 2D building blocks in artificial heterostructures, [4,5] as electron transport materials in solar cells [3d] and photocatalysts, [3a-c] or as ultrathin high-k capacitors or gate insulators. [2] Following pioneering work by Sasaki and Mallouk on the exfoliation and utilization of 2D oxide nanosheets, [1a-c,6] Osterloh and co-workers demonstrated the vast potential of calcium niobate nanosheet suspensions in photocatalytic water splitting. [3a,b] While the large-band gap Ca 2 Nb 3 O 10 À semiconductor nanosheets (E g = 3.5-3.6 eV) [3a, 7] produce hydrogen from pure water, the decomposition of n-tetrabutylammonium (TBA), which is commonly used as an exfoliation agent, is another fingerprint of the photoactivity of calcium niobate under UV-illumination in air.[3b] Similar observations for titania nanosheets modified with organic cations were reported by Sasaki and co-workers earlier.[8] This photodegradation of organic counterions was later used to pattern graphene oxide/PDDA/titania multilayer or titania thin films on the millimeter or hundreds of micron scale, respectively,u sing as hadow mask.[9] However,b eing able to precisely sculpture nanosheet architectures with feature sizes smaller than 100 microns is highly desired for applications in integrated microelectronic circuits due to the ever increasing need for miniaturization.[2b, 10] Recent attempts to pattern nanosheet thin films on the mm-scale were based on MoS 2 , [10] reduced graphene oxide (rGO), [11] or graphene oxide (GO).[12] In these approaches the patterns are either obtained by laser patterning or by electrochemical microstamping. [10][11][12] However,n one of these latter methods utilizes the intrinsic properties of the nanosheets for pattern creation, and all...