search within this otherwise embarrassingly rich reservoir, via soundly established molecular engineering guidelines at both molecular and macroscopic material scale. Their resulting higher nonlinear coeffi cients, [ 3 ] as well as their inherently low dielectric constant further points out the interest of this family of materials. Whereas poled polymers provide the advantage of an eased fabrication for large areas fi lms with mechanical fl exibility of interest for some applications, the dilution and inherent statistical disorder of the embedded nonlinear dyes are a price to pay, which make organic crystals worthy of attention for complementary reasons. Indeed, their growth is more laborious and still an active domain of research, but they cannot be matched in terms of their optimal compaction [ 4 ] due to the absence of dilution of molecular units in crystalline structures. Moreover, their frozen structure resulting from an interplay between intermolecular forces, ensures better stability then that of externally poled structures which are prone to the relaxation of the average molecular orientation with time. In the wake of these advantages, research on quadratic nonlinear organic crystals, including electrooptic ones, has remained an active area, all the way to sophisticated devices such as high Q ring modulators. [ 5 ] Moreover, thin fi lm formatting and the related growth processes have attracted particular interest in view of ultrafast applications [ 6 ] and more recently of Terahertz generation or detection. [ 7 ] Whereas such materials as 4-N , N -dimethylamino-4′-N ′-methyl-stilbazolium tosylate which belongs to the subclass of organic molecular salts [ 8 ] has been shown to reach fi gures of merits of a few hundreds of pm V −1 , MNA (2-methyl-4-nitroaniline) has been an early-on and quite successful candidate, which is a direct spin-off from the basic para-nitroaniline (pNA) molecular diode template, which has served as the main pool for nonlinear structures since the seventies. Whereas a wealth of fundamental and more applied studies had been devoted throughout the eighties and nineties to this class of materials and properties, a revival has been experienced from the end of the last century as a result of the advent of nanophotonics and the need to develop new nanoscale nonlinear crystals and labels for physics and biophysics, among which molecular nanocrystals appear as natural "second-generation" candidates. [ 9 ] In parallel, new characterization and imaging techniques capable to follow up with the downscaling of materials and to allow for their characterization, [ 10 ] bothThe recently proposed Pockels linear electrooptical microscopy is being applied to a quality and performance characterization of the 2-methyl-4-nitroaniline quadratic nonlinear optical molecular crystal down to confocal microscope resolution. Samples are grown between electrodes in single-fi lm format. The dominant electrooptic tensor coeffi cient is determined and the distribution of the electric fi eld is mapped so as to ch...