MRI estimation of cerebral blood volume (CBV) is useful in mapping potential brain function. To obtain high-resolution CBV maps, it typically requires intravenous (IV) injections of Gadolinium-based contrast agents (GBCAs), the use of which has come under new scrutiny. Here, we design and implement a deep learning algorithm, DeepContrast, to estimate GBCA contrast directly from T1-weighted (T1W) structural MRI. The predicted contrast performs equally well as the GBCA-enhanced CBV map even in mapping subtle age-related functional changes in the human brain. Therefore, our study demonstrates the feasibility of substituting GBCA in human brain MRI using DeepContrast.