The stability of nonpatterned and nanopatterned strong polyelectrolyte brushes (PEBs) is studied as a function of both brush character and the properties of a contacting liquid. High-molecularweight PEBs of poly(4-methyl vinylpyridinium iodide) (PMeVP) are synthesized using surface-initiated radical-chain polymerization. Nanopatterned brushes (NPBs) line with pattern sizes ranging from 50 to 200 nm are generated by patterning the initiator layer using deep-ultraviolet photolithography followed by brush growth initiated from the patterned layer. Homogeneous PEBs with different degrees of charging and grafting densities are exposed to water and salt solutions with different temperatures for different periods. The degradation is monitored through dry-state ellipsometry and atomic force microscopy measurements. Enhanced degrafting for more strongly swollen polymer brushes can be observed in agreement with an "entropic spring" model. Based on the results of the nonpatterned brushes, the NPBs are exposed to water at different temperatures and external salt content for varying periods of time. Counterintuitively, the NPBs show increased degrafting for smaller patterns, which is attributed to different polymer chain dynamics for nanobrushes and microbrushes. We investigate the influence of thermodynamic and kinetic parameters on the stability of (nanopatterned) PEBs and discuss the role of entanglements and formation of complexes in such films.The additional strong electrostatic interactions due to the charges are a reason for the unusual and versatile behavior of PEBs compared to their neutral peers. 12 Thus, if polymer brushes with similar structures are compared, while neutral polymer brushes can already stretch by up to 40% of their contour length, PELs can stretch even more and stretched values of more than 65% of the contour length have been observed. 13 Such strong stretching leads to a significant loss of entropy and completely changes the properties of the layers, rendering PEBs as an attractive molecular architecture. They are often used for applications in the field of biochemistry as most organic molecules synthesized by living organisms carry electrolyte groups themselves. Thus, PEBs have been used for the analysis and study of proteins, 14 DNA, 15 vitamins 16 and in gene, 16 and drug 17 delivery. In addition, they are also perfect candidates for applications in antifouling medical devices, 18 biosensing, 19 antibacterial coatings, 5 cell culture substrates, 20 stem cell Additional supporting information may be found in the online version of this article. † M. Menzel and W. -L. Chen contributed equally to this article.