Pre-Quaternary terrestrial climate variability is less well understood than that during the Quaternary. The continuous eolian Red Clay sequence underlying the well-known Quaternary loess-paleosol sequence on the Chinese Loess Plateau (CLP) provides an opportunity to study pre-Quaternary terrestrial climate variability in East Asia. Here, we present new mineral magnetic records for a recently found Red Clay succession from Shilou area on the eastern CLP, and demonstrate a marked East Asian climate shift across the Miocene-Pliocene boundary (MPB). Pedogenic fine-grained magnetite populations, ranging from superparamagnetic (SP)/single domain (SD) up to small pseudo-single domain (PSD) sizes (i.e., from <30 nm up to ~1000 nm), dominate the magnetic properties. Importantly, our mineral magnetic results indicate that both pedogenic formation of SP grains and transformation of SP grains to SD and small PSD grains accelerated across the MPB in the Shilou Red Clay, which are indicative of enhanced pedogenesis. We relate this enhanced pedogenesis to increased soil moisture availability on the CLP, associated with stronger Asian Summer Monsoon precipitation during an overall period of global cooling. Our study thus provides new insights into the Miocene-Pliocene climate transition in East Asia.