This PDF file includes:

• Supplementary Materials and Methods
• Fig. S1. Simulated dependence of R2free and ΔR₂ on internal correlation time τ_i and S² order parameter.
• Fig. S2. Range of validity of Eq. 3 for the extraction of S² from ΔR₂.
• Fig. S3. Experimental ¹⁵N spin relaxation parameters of Im7 in the absence of NPs.
• Fig. S4. Experimental ¹⁵N spin relaxation parameters of CBD1 in the absence of NPs.
• Fig. S5. Comparison between NMR S²(ΔR₂) and x-ray B-factors of backbone nitrogen atoms in crystal structures.
• Fig. S6. Dependence of ΔR₂ values on SNP concentration.
• Fig. S7. Mapping of experimental S²(ΔR₂) onto the structural model of Im7 when bound to the DNase domain of colicin E7.
• References (49–63)

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