We demonstrate that thin metallic glasses of VxZr100-x, deposited by direct current magnetron sputtering, closely approximate the structural characteristics of theoretically predicted maximally amorphous materials. Experimentally, x-ray reflectometry reveals atomically flat films with well-defined thickness and low surface roughness, while Rutherford backscattering spectrometry confirms V/Zr stochiometry within 1 at.% and a compact, systematically varying density with composition. Transmission electron microscopy shows no evidence of columnar growth, consistent with fully amorphous and homogeneous films. Using ab initio stochastic quenching to generate representative maximally amorphous configurations, we find excellent agreement with experiment in terms of mass density and pair distribution functions. The calculated structures are mechanically stable, elastically isotropic, and exhibit high Poisson ratios and Pugh ratios indicating a characteristically ductile response. The combination of compactness and ductility suggests potential for applications in mechanically resilient coatings and for hydrogen storage, where deformation tolerance and structural integrity are critical. The agreement between simulation and experiment across structural and compositional descriptors supports the conclusion that sputtered V-Zr metallic glasses can be viewed as experimental realizations of statistically maximally amorphous states within the framework of the random valley approximation. We propose such structures can serve as well defined benchmarks for the maximal degree of amorphousness.