Quantification of brain function is a significant milestone towards understanding of the underlying workings of the brain. Photoacoustic (PA) imaging is the emerging brain sensing modality by which the molecular light absorptive contrast can be non-invasively quantified from deep-lying tissue (~several cm). In this BRAIN initiative effort, we propose high-speed transcranial PA imaging using a novel, compact pulsed LED illumination system (Prexion Inc., Japan) with 200-uJ pulse energy for 75-ns duration, and pulse repetition frequency (PRF) up to 4kHz at near-infrared (NIR) wavelengths of 690-nm and 850-nm switchable in real-time. To validate the efficacy of the proposed system, preliminary ex vivo experiments were conducted with mice skull and human temporal bone, which included vessel-mimicking tubes filled with 10% Indian Ink solution and light absorptive rubber material, respectively. The results indicated that significant PA contrast, 150% signal-to-noise ratio (SNR), can be achieved through the mice skull only with 64 subsequent frame averaging. The minimal number of frames for averaging required was only 16 to generate signal above background noise, leading to 250 Hz frame rate in the strictest temporal frame separation. Furthermore, distinguishable PA contrast was achieved with human temporal bone with 64-frame averaging. Overall, the preliminary results indicate that the LED illumination system can be a cost-effective solution for high-speed PA brain imaging in preclinical and clinical applications, compared to expansive and bulky Nd:YAG laser systems commonly used in PA imaging.