Surgical resection (SR) following transarterial chemoembolization (TACE) is a promising treatment for unresectable hepatocellular carcinoma (uHCC). However, biomarkers for the prediction of postoperative recurrence are needed. To develop and validate a model combining deep learning (DL) and clinical data for early recurrence (ER) in uHCC patients after TACE. A total of 511 patients who received SR following TACE were assigned to derivation (n = 413) and validation (n = 98) cohorts. Deep learning features were taken from the largest tumor area in liver MRI. A nomogram using DL signatures and clinical data was made to forecast early recurrence risk in uHCC patients. Model performance was evaluated using area under the curve (AUC). A total of 2278 subsequences and 31,346 slices multiparametric MRI including contrast-enhanced T1WI, T2WI and DWI were input in the DL model simultaneously. Multivariable analysis identified three independent predictors for the development of the nomogram: tumor number (hazard ratio [HR]:3.42, 95% confidence interval [CI]: 2.75-4.31, P = 0.003), microvascular invasion (HR: 9.21, 6.24-32.14; P < 0.001), and DL scores (HR: 17.46, 95% CI: 12.94-23.57, P < 0.001). The AUC of the nomogram was 0.872 and 0.862 in two cohorts, significantly outperforming single-subsequence-based DL mode and clinical model (all, P < 0.001). The nomogram provided two risk strata for cumulative overall survival in two cohorts, showing significant statistical results (P < 0.001). The DL-based nomogram is essential to identify patients with uHCC suitable for treatment with SR following TACE and may potentially benefit personalized decision-making.