Stroke is the third-leading cause of death and disability, and poststroke falls (PSF) are common at all stages after stroke and could even lead to injuries or death. Brain information from functional near-infrared spectroscopy (fNIRs) may precede conventional imaging and clinical symptoms but has not been systematically considered in PSF risk prediction. This study investigated the difference in brain activation between stroke patients and healthy subjects, and this study was aimed to explore fNIRs biomarkers for early screening of PSF risk by comparing the brain activation in patients at and not at PSF risk. In this study, we explored the differences in brain activation and connectivity between stroke and healthy subjects by synchronizing the detection of fNIRs and EMG tests during simple (usual sit-to-stand) and difficult tasks (sit-to-stand based on EMG feedback). Thereby further screened for neuroimaging biomarkers for early prediction of PSF risk by comparing brain activation variability in poststroke patients at and not at fall risk during simple and difficult tasks. The area under the ROC curve (AUROC), sensitivity, and specificity were used to compare the diagnostic effect. A total of 40 patients (22 not at and 18 at PSF risk) and 38 healthy subjects were enrolled. As the difficulty of standing task increased, stroke patients compared with healthy subjects further increased the activation of the unaffected side of supplementary motor area (H-SMA) and dorsolateral prefrontal cortex-Brodmann area 46 (H-DLFC-BA46) but were unable to increase functional connectivity (Group*Task: p < 0.05). More importantly, the novel finding showed that hyperactivation of the H-SMA during a simple standing task was a valid fNIRs predictor of PSF risk [AUROC 0.74, p = 0.010, sensitivity 77.8%, specificity 63.6%]. This study provided novel evidence that fNIR-derived biomarkers could early predict PSF risk that can facilitate the widespread use of real-time assessment tools in early screening and rehabilitation. Meanwhile, this study demonstrated that the higher brain activation and inability to increase the brain functional connectivity in stroke patients during difficult task indicated the inefficient use of brain resources.