Proteorhodopsin (PR), a membrane protein with highly degenerated amino acid type and Maltose Binding Protein (MBP) as an example of large molecular-weight protein (~42 kDa). For PR, we found that 47.7 % of the shifts for all the Hamide, Namide and Cα were correctly assigned with the same protocol shown above for GB1 (Table and Figure ). The rate of correct assignment is limited by the Cα chemical shift degeneration (Figure ). However, adding only one peak list generated from the hNcocaNH data improved the success rate to 92.3 %. The latter data can be readily acquired for T2-limited samples using dipolar coupling based Cα/C' magnetization transfer , and proposed as a part of the default dataset. When the conventional CANH/CAcoNH data are combined with hNcocaNH, the rate of correct assignment remained 60.6 %. These results indicate that the residue type information derived from the BE-CANH/CAcoNH experiments is critical for a successful sequential assignment. For MBP, the success rate was 77.9 % using the proposed three datasets, and the introduction of the BEexperiments improved the rate similarly to the case for PR (Table and Figure , S10). Thus, our proposed BE-experiments can provide a powerful basis for the challenging proteins.