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Purpose  To develop a method for rapid sub‐millimeter T 1 , T 2 ,T  2  *    $$ {\mathrm{T}}_2^{\ast } $$   , and QSM mapping in a single scan using multi‐contrast learned acquisition and reconstruction optimization (mcLARO).    Methods  A pulse sequence was developed by interleaving inversion recovery and T 2  magnetization preparations and single‐echo and multi‐echo gradient echo acquisitions, which sensitized k‐space data to T 1 , T 2 ,T  2  *    $$ {\mathrm{T}}_2^{\ast } $$   , and magnetic susceptibility. The proposed mcLARO optimized both the multi‐contrast k‐space under‐sampling pattern and image reconstruction based on image feature fusion using a deep learning framework. The proposed mcLARO method withR  =  8   $$ R=8 $$    under‐sampling was validated in a retrospective ablation study and compared with other deep learning reconstruction methods, including MoDL and Wave‐MoDL, using fully sampled data as reference. Various under‐sampling ratios in mcLARO were investigated. mcLARO was also evaluated in a prospective study using separately acquired conventionally sampled quantitative maps as reference standard.    Results  The retrospective ablation study showed improved image sharpness of mcLARO compared to the baseline network without the multi‐contrast sampling pattern optimization or image feature fusion module. The under‐sampling ratio experiment showed that higher under‐sampling ratios resulted in blurrier images and lower precision of quantitative values. The prospective study showed that small or negligible bias and narrow 95% limits of agreement on regional T 1 , T 2 ,T  2  *    $$ {\mathrm{T}}_2^{\ast } $$   , and QSM values by mcLARO (5:39 mins) compared to reference scans (40:03 mins in total). mcLARO outperformed MoDL and Wave‐MoDL in terms of image sharpness, noise suppression, and artifact removal.    Conclusion  mcLARO enabled fast sub‐millimeter T 1 , T 2 ,T  2  *    $$ {\mathrm{T}}_2^{\ast } $$   , and QSM mapping in a single scan.

mcLARO : Multi‐contrast learned acquisition and reconstruction optimization for simultaneous quantitative multi‐parametric mapping