Magnetic grain-size variations have been used as sensitive paleoclimate proxies to investigate the evolution of the East Asian summer monsoon, but their relationship with temperature and precipitation is not entirely clear. Here we find that two magnetic grain-size proxy records (χARM/χLF and χARM/SIRM, where χARM, χLF and SIRM are anhysteretic remanent magnetization susceptibility, magnetic susceptibility measured at 470 Hz and saturation isothermal remanent magnetization, respectively) of Chinese loess and red-clay sediments co-vary during the last 6 Ma, except between ~ 4.5 and 2.6 Ma, when these two records had opposite trends. We attribute this disparate behavior to the different responses of χARM/χLF and χARM/SIRM to temperature and precipitation during ~ 4.5–2.6 Ma, when temperature and precipitation on the Chinese Loess Plateau were decoupled. A comparison of the loess and red-clay χARM/χLF and χARM/SIRM records with the global ice-volume proxy records reveals that χARM/χLF is more sensitive to temperature variations than χARM/SIRM. The results suggest that temperature on the Chinese Loess Plateau had a cooling trend from ~ 4.5 to ~ 2.6 Ma, whereas rainfall tended to increase. Our studies demonstrate that joint analysis of loess χARM/χLF and χARM/SIRM records can reveal paleoclimatic information that cannot be revealed by a single parameter.