The Irish-born actor is in the Capital filming Will Ferrell's new Netflix comedy Eurovision.
And after a day's filming, the GoldenEye star was taken aback by the city's skyline.
"Edinburgh Castle in the golden glow of day’s end, crowned by a rainbow," Brosnan, 66, posted with a photo on Instagram.
Leading stars Ferrell and Rachel McAdams have been spotted on Edinburgh’s landmarks, Arthur’s Seat and Calton Hill as filming began earlier in the week.
The two play Icelandic singers who are given the opportunity to perform at the famous song contest when it was held in the Scottish Capital in 1972.
Ferrell, 52, was seen on Arthur’s Seat wearing bright yellow overalls and matching jacket over a plaid shirt while sporting long, damp hair.
McAdams, 40, was also seen on location wearing a pink and white jacket, maroon trousers and a black and white striped jumper with her blonde hair knotted.
Filming will continue around the city centre until the middle of next week.