One major public health issue is cancer chemotherapy; despite constant progress in the area, administration of anticancer drugs to patients is often associated with serious side effects. It is therefore imperative to develop vehicles for encapsulation and controlled delivery of such drugs. Anticancer drugs include small peptide drugs, such as Bortezomib (BTZ). Self-assembling peptides have been recently reported as promising drug delivery agents. The research reported here proposes the encapsulation of BTZ into peptide hydrogels formed by the self-assembling FmocFF dipeptide as delivery vehicle. We selected FmocFF as an encapsulation vehicle based on our previous simulation study on the complexation propensity of Bortezomib (BTZ) with various peptide gelators. Herein we undertook additional computational studies that highlight the benefits of FmocFF as a potential effective nanocarrier for BTZ combined with experiments of encapsulation and evaluation of BTZ release. Based on these computational and experimental results, we propose the Fmoc-FF dipeptide hydrogel as a promising matrix for the controlled delivery of BTZ.