A technique for combined time‐of‐flight (TOF) MR angiography (MRA) and quantitative susceptibility mapping (QSM) was developed with key features of standard three‐dimensional (3D) TOF acquisitions, including multiple overlapping thin slab acquisition (MOTSA), ramped RF excitation, and venous saturation. The developed triple‐echo 3D TOF‐QSM sequence enabled TOF‐MRA, susceptibility‐weighted imaging (SWI), QSM, and R2* mapping. The effects of ramped RF, resolution, flip angle, venous saturation, and MOTSA were studied on QSM. Six volunteers were scanned at 3 T with the developed sequence, conventional TOF‐MRA, and conventional SWI. Quantitative comparison of susceptibility values on QSM and normalized arterial and venous vessel‐to‐background contrasts on TOF and SWI were performed. The ramped RF excitation created an inherent phase variation in the raw phase. A generic correction factor was computed to remove the phase variation to obtain QSM without artifacts from the TOF‐QSM sequence. No statistically significant difference was observed between the developed and standard QSM sequence for susceptibility values. However, maintaining standard TOF features led to compromises in signal‐to‐noise ratio for QSM and SWI, arising from the use of MOTSA rather than one large 3D slab, higher TOF spatial resolution, increased TOF background suppression due to larger flip angles, and reduced venous signal from venous saturation. In terms of vessel contrast, veins showed higher normalized contrast on SWI derived from TOF‐QSM than the standard SWI sequence. While fast flowing arteries had reduced contrast compared with standard TOF‐MRA, no statistical difference was observed for slow flowing arteries. Arterial contrast differences largely arise from the longer TR used in TOF‐QSM over standard TOF‐MRA to accommodate additional later echoes for SWI. In conclusion, although the sequence has a longer TR and slightly lower arterial contrast, provided an adequate correction is made for ramped RF excitation effects on phase, QSM may be performed from a multiecho sequence that includes all key TOF features, thus enabling simultaneous TOF‐MRA, SWI, QSM, and R2* map computation.