This work proposes a facile fabrication strategy for thermally conductive graphite nanosheets/poly(lactic acid) sheets with ordered GNPs (o-GNPs/PLA) via fused deposition modeling (FDM) 3D printing technology. Further combinations of o-GNPs/PLA with Ti 3 C 2 T x films prepared by vacuum-assisted filtration were carried out by “layer-by-layer stacking-hot pressing” to be the thermally conductive Ti 3 C 2 T x /(o-GNPs/PLA) composites with superior electromagnetic interference shielding effectiveness (EMI SE). When the content of GNPs was 18.60 wt% and 4 layers of Ti 3 C 2 T x (6.98 wt%) films were embedded, the in-plane thermal conductivity coefficient ( λ || ) and EMI SE (EMI SE || ) values of the thermally conductive Ti 3 C 2 T x /(o-GNPs/PLA) composites significantly increased to 3.44 W·m –1 ·K –1 and 65 dB (3.00 mm), increased by 1223.1% and 2066.7%, respectively, compared with λ || (0.26 W·m –1 ·K –1 ) and EMI SE || (3 dB) of neat PLA matrix. This work offers a novel and easily route for designing and manufacturing highly thermally conductive polymer composites with superior EMI SE for broader application.