We report on the scalable synthesis and characterization of novel architecture three-dimensional high-capacity amorphous Silicon Nanostructures (SiNSs)-based anodes, with focus on studying their electrochemical degradation mechanisms. By using our novel, low cost and high mass loading chemical vapor deposition (CVD) procedure we synthesized anodes that have shown stable cycle life for many hundreds of cycles and provided capacities of up to 5.5mAh/cm2, very low irreversible capacity and good compatibility with commercial cathodes such as NCA and LFP. Our state-of-the-art anodes have been coupled with commercial cathodes not only for proof of concept but also for the study of the degradation mechanisms of full cells. The correlation between the degradation of the anode and the cathode is demonstrated with the use of three-electrode cells. Notably, it was found that the growth of the solid electrolyte interphase (SEI) thickness and resistivity represents the major reason for the observed capacity loss of the SiNSs-based anodes. Most recently, these anodes have successfully been incorporated in industrial hardware cylindrical cells, proving they are a viable candidate for anodes of the next generation lithium ion batteries for mobility and portable applications.