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Cook, who turned 33 on Christmas Day, also became the first Englishman to score more than 200 at the MCG and overtook another West Indies champion — Viv Richards — in posting the biggest ever score by a visiting player at the iconic ground.
His mammoth total this Test comes after a lacklustre series to date which had yielded just 83 runs combined from six innings with a top score of 37 in Adelaide.
This innings has drawn comparisons to Cook's 2010-11 Ashes series in Australia, when he carved up the locals with mammoth knocks of 235no, 148 and 189.
Cook said that series was a distant memory but after a tough tour to date it been rewarding to put runs on the board.
"I can't remember that far back to be honest with you," he said.
"Obviously with my batting over a period of time there's quite a few moving parts to it. When they're not quite in synch it can be quite frustrating and basically the one way of delivering it is time in the middle and if you get time in the middle and you feel at ease sometimes I play quite nicely.
"I always feel as though I've got the backing of the selectors but you've still got to deliver the goods and I hadn't done that on this tour and it was frustrating, very frustrating.
Highest Run-scorers in Test Cricket
Updated end of day three during 4th Ashes test
15,921_Sachin Tendulkar, India (200 tests)
13,378_Ricky Ponting, Australia (168)
13,289_Jacques Kallis, South Africa (166)
13,288_Rahul Dravid, India (164)
12,400_Kumar Sangakkara, Sri Lanka (134)
11,956_x-Alastair Cook, England (151)
11,953_Brian Lara, West Indies (131)
11,867_Shivnarine Chanderpaul, West Indies (164)
11,814_Mahela Jayawardene, Sri Lanka (149)
11,174_Allan Border, Australia (156)
10,927_Steve Waugh, Australia (168)
10,122_Sunil Gavaskar, India (125)
10,099_x-Younis Khan, Pakistan (118)