Recently, the near-infrared-II (NIR-II, 1000–1350 nm) region has been extensively applied in deep-tissue photothermal therapy (PTT) on account of it having stronger tissue penetration and a higher maximum permissible exposure (MPE) than the near-infrared-I (NIR-I, 650–950 nm) region. In this study, we developed a rapid and convenient in situ polymerization strategy to fabricate polypyrrole nanosheets (PPy NSs) within a few minutes using manganese dioxide nanosheets (MnO₂ NSs) as both the oxidant and the self-sacrificed template. The fabricated PPy NSs exhibited excellent NIR-II absorption, which conferred its high photothermal conversion efficiency (66.01%) at 1064 nm and its photoacoustic (PA) imaging capability. Both in vivo and in vitro studies have shown that that PPy NSs possess good biological safety and excellent PTT efficacy and PA imaging performances. Thus, the as-synthesized PPy NSs could effectively achieve PA imaging-guided photothermal tumor ablation under 1064 nm excitation. Our work provides a novel and promising method for the rapid preparation of PPy NSs without the addition of exogenous oxidants and subsequent template removal, which could be regarded as potential photothermal agents (PTAs) to integrate the diagnosis and treatment of cancer.