The return of straw is a widely used agricultural practice for increasing the soil organic carbon (SOC) content and improving soil structure in Mollisols, owing to the decline caused by continuous high-intensity tillage. We conducted a field experiment where corn straw was continuously returned for 10 years to investigate effects of the straw on the size distribution and stability of soil aggregates and on SOC density fractions. The treatments were no straw return (CK) and four rates of straw return: 6000 kg hm⁻² (S1), 9000 kg hm⁻² (S2), 12,000 kg hm⁻² (S3), and 15,000 kg hm⁻² (S4). SOC contents after straw return for bulk soil, a free light fraction (F-LF), an occluded light fraction (O-LF), and a heavy fraction (HF) were significantly higher by 27.0, 644.3, 720.0, and 69.2%, respectively, in S4 than CK. The contents of F-LF, O-LF, and HF in aggregates >2.00 mm were significantly higher by 194.2, 162.1, and 35.8%, respectively, in S4 than CK. Structural equation modeling indicated that SOC contents and aggregates >0.25 mm were directly correlated with the amount of straw returned. We conclude that returning 15,000 kg m⁻² of straw would be an effective agronomic practice to restore Mollisol fertility.