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The mechanism behind the 1H nuclear magnetic resonance (NMR) frequency dependence of T1 and the viscosity dependence of T2 for polydisperse polymers and bitumen remains elusive. We elucidate the matter through NMR relaxation measurements of polydisperse polymers over an extended range of frequencies (f0 = 0.01-400 MHz) and viscosities (η = 385-102 000 cP) using T1 and T2 in static fields, T1 field-cycling relaxometry, and T1ρ in the rotating frame. We account for the anomalous behavior of the log-mean relaxation times T1LM ∝ f0 and T2LM ∝ (
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