We evaluated the liver transplantation (LT) criteria in acute-on-chronic liver failure (ACLF), incorporating an urgent living-donor LT (LDLT) program. Critically ill patients with a Chronic Liver Failure-Consortium-ACLF score (CLIF-C_ACLF_score)≥65, previously considered unsuitable for LT, were included to explore the mortality threshold of the CLIF-C_ACLF_score (CLIF-C_ACLF_score_threshold). We followed 854 consecutive patients with ACLF (276 ACLF-2 and 215 ACLF-3) over 10 years among 4432 LT recipients between 2008 and 2019. For advanced ACLF patients without immediate deceased-donor (DD) allocation, an urgent LDLT program was expedited. The CLIF-C_ACLF_score_threshold was determined by the metrics of transplant survival benefit: >60% 1-year and >50% 5-year survival rate. In predicting post-LT mortality, the CLIF-C_ACLF_score outperformed the MELD-Na and MELD-3.0 scores but was comparable to the Sundaram ACLF-LT-mortality (SALT-M) score. A CLIF-C_ACLF_score≥65 (n=54) demonstrated post-transplant survival benefits, with 1-year and 5-year survival rates of 66.7% and 50.4% (P<0.001). Novel CLIF-C_ACLF_score_threshold for 1-year and 5-year mortalities was 70 and 69, respectively. A CLIF-C_ACLF_score-based nomogram for predicting survival probabilities, integrating cardiovascular disease, diabetes, and donor type (LDLT vs. DDLT), was generated. This study suggests reconsidering the criteria for unsuitable LT with a CLIF-C_ACLF_score≥65. Implementing a timely salvage LT strategy, incorporating urgent LDLT, can enhance survival rates.