Fabrication of self-assembled structures using multiple building blocks with diverse functionalities such as biomolecules, polymers and inorganic nanoparticles has attracted considerable interest due to the potential applications of hybrid constructs in biotechnology and bio-electronic devices. [1,2] A principal candidate biomolecule for incorporation into multi-functional devices is the photoactive protein-retinal complex, bacteriorhodopsin (BR), [3] which acts as a light-activated proton pump in the purple membrane (PM) of halophilic bacteria. Extracted PM fragments exhibit photoelectric, photochromic and photo-induced proton transport properties, and have been investigated as potential materials for holography, non-linear optics, and optical information processing. [3,4] PM films are only stable over a limited range of pH, humidity and temperature conditions, and are fragile and difficult to manipulate, which severely limit their application in photoelectric devices. PM fragments can be readily extracted from halophilic bacteria such as Halobacterium salinarum in the form of micronsized, 5 nm-thick lipid bilayer sheets that consist of a 2D protein/lipid crystalline array of unidirectionally oriented BR molecules. Proton transport from the cytoplasmic to extracellular side of the PM is initiated by light-activated isomerisation of the BR-bound retinal chromophore, and coupled with a thermally activated photocycle involving a series of spectroscopic intermediates (J, K, L, M, N, and O states) associated with deprotonation/protonation of the Schiff-base retinal linkage. A significant blue shift occurs between the protonated ground state (B 568 ) and stable unprotonated intermediate (M 412 ) that gives rise to photochromism and the possibility of using PM patches in imaging and recording devices such as photochromic inks, holographic interferometry and volumetric memories.[4] The response to steady state illumination is extremely sensitive and the photocycle can be cycled many times more than for synthetic materials, as well as enhanced in efficiency by increasing the M lifetime by site-directed mutagenesis (notably replacing Asp96 by Asn96). [4,5] Previous research has been undertaken on the incorporation of PM flakes into polymer gels [6,7] and sol-gel derived glasses [8][9][10][11][12] in order to produce bulk composite materials for potential photochromic applications. In contrast, the photoelectric response of BR, which depends on a net charge separation (voltage) across the lipid membrane, necessitates the fabrication of films in which PM fragments are uniformly oriented in order to facilitate unidirectional proton transport. Several approaches, involving layer by layer deposition, [13][14][15] Langmuir-Blodgett deposition, [16][17][18][19] electrophoretic sedimentation, [20,21] antibody recognition [22] and chemiadsorption selfassembly [23] have been developed to achieve this objective.The films are generally soft and brittle, and the photoelectric response sensitive to changes in environmental conditions...