The South African ace, appearing in his second World Championship, produced the performance of his career to follow up a 4-3 preliminary round win over Portugal's Jose de Sousa earlier on Wednesday with victory over the number 29 seed.
Bristol's Brown was 2-0 up in the deciding set and missed one match dart at the bullseye before Petersen won the match in dramatic style with four straight legs to set up a last 32 clash against Gary Anderson.
Brown made a good start to the match by breaking his opponent's throw to take the first leg before hitting double top at the first attempt to win the second.
The Bristol man then won the third leg to take an early lead before Petersen hit double ten to win his first leg of the match at the start of the set two.
Brown, who lost to Terry Jenkins in last year's tournament, hit double two to take the next leg and landed double top to take the third.
The South African hit double three with a pressure last dart to take the fourth leg and then produced an excellent 13-dart finish to take the set and level the match.
Brown hit double 12 to win the first leg of set three against the darts but Petersen hit back immediately with a clinical 120 finish.
The South African took out 76 to win the third leg before Brown hit an impressive 13-darter to take the fourth.
Petersen held advantage of throw in the deciding leg and, with the aid of a 180, left 54 after 15 darts only to see Brown finish a 130 checkout on the bullseye to snatch the set.
Petersen put that disappointment behind him to break throw at the start of the fourth set, before landing double 16 to take the second leg.
The South African then missed a dart at bullseye for the set in the third leg, and Brown hit double top at the first attempt to hit back.
Brown, though, missed double 16 for a 131 checkout in the fourth leg and Petersen hit double 17 to send the match into a fifth set.
The Bristol player made a good start in the first leg by hitting double top at the first time of asking, and the second soon followed as he moved a leg away from victory.
Petersen hit tops to claim the third leg, and hit a superb 80 finish to win the fourth after Brown missed a dart at the bullseye to take the match.
Petersen then won his third successive leg by hitting double top with his first dart, and secured victory in the next by landing a pressure double nine with his third dart.
"It's a great feeling to win, unbelievable and just crazy," admitted Petersen. "It's been a boyhood dream of mine to play in the Ladbrokes World Championship and last year was a new thing for me to be around these great players.
"This year was a bit different because I'm used to playing the other players and I have more experience but it's a dream come true. I'm sure I have more in me
"I'm buzzing for the second round. Gary is an awesome player and the Premier League champion but it's a game of two warriors battling it out, and whoever's sword is the sharpest and who moves the quickest wins.
"On reputation, he's brilliant but on stage that counts for nothing. If your doubles don't go in you can go out and I could be through to the last 16."
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