An experiment was conducted from 2013 to 2015 in three reddish paddy fields under different nutrient levels to comprehensively evaluate the effects of different fertilization modes on available nutrient contents and rice yields in order to find the best fertilization mode. The tested fields were located respectively in Beisheng, Lotus and Dahu towns in Liuyang, eastern Hunan. The fertilization modes included CK, no-fertilizer; CF, conventional fertilizer; NPKG, 60% chemical fertilizer + 40% organic manure (straw + astragalus smicus, equivalent nitrogen substitution); and NPK, single chemical fertilizer. The results showed that compared with CK, other fertilization modes significantly increased rice biological yield, NPKG mode was the best and in which rice biomass yield showed a continuous increasing trend. Compared with CK, NPK and CF modes, rice yields under NPKG mode were increased 38.3%-62.4%, 1.7%-9.6% and 8.4%-12.0% respectively by promoting the number of productive ear and seeds per ear. The contents of rapid available nutrients in soils under NPKG mode showed an increasing trend and were significantly higher than those of other fertilization modes, while the contents of rapid available nutrients in soils under CF mode decreased gradually. From the aspect of crop yield, the proportion of chemical fertilizer in NPKG mode should be increased in the low fertility area, but the proportion of organic manure should be increased from the long term in terms of promoting soil fertility, while for the middle-high fertility area, the proportion of organic fertilizer should be increased gradually. Non-fertilization will decrease but fertilization increase soil available nutrients, in which NPKG mode is optimal in promoting soil fertility and rice yield.