Previous studies have shown that high-arousal positive and negative facial expressions influence event-related potential (ERP) and time-frequency responses depending on attentional focuses. However, little is known about how relevant neural responses are influenced by surprised facial expressions, which are also high in arousal but ambiguous in valence. To address the issue, 38 participants were presented with surprised, happy, angry and neutral facial expressions. Attention was manipulated to focus on facial emotional attributes, facial non-emotional attributes, non-facial attributes, or was free to the participants. ERP results showed larger N170 responses to surprised compared to neutral facial expressions when attention focused on facial attributes and to surprised compared to angry and neutral facial expressions when attention focused on facial non-emotional attributes. Time-frequency analyses revealed reduced power of early occipital theta to surprised compared to happy and angry expressions when attention focused on facial emotions and to surprised compared to angry expressions when attention focused on non-facial stimuli. Parietal delta power was smaller for surprised facial expressions than for angry facial expressions when attention focused on facial emotions and for surprised facial expressions than for angry and neutral facial expressions when attention was directed to non-facial stimuli. These findings might suggest that neural responses to surprised facial expressions are modulated by attentional focus.