Storey joined Baroness Tanni Grey-Thompson as Britain's most successful female Paralympian with a dominant performance to triumph in the 64km race, securing her fourth gold at London 2012.
The 34-year-old, who won her first title as a 14-year-old swimmer in Barcelona in 1992 and her 10th in the C5 Time Trial yesterday, attacked from the start of the eight-lap event and finished in 1:40:36.
In taking her Paralympic gold medal total to 11 - and 22 medals in all - Storey equalled Grey-Thompson and swimmer David Roberts' haul. Mike Kenny won 16 gold medals as a swimmer from 1976 to 1988.
Anna Harkowska finished in the silver medal position, with Kelly Crowley taking bronze.
'It's just amazing,' said Storey. 'This has been the greatest Games for me. I won two gold medals in Barcelona, three in Atlanta, two in Beijing. I've won four here - I can't get over it.
'I wanted to put in my very best performance today and finish off the job I set out to do at the beginning of the week.
'I wanted to win every race and the outcome of that has been four gold medals, but you have to stay focused on the process that you've got to do and every race has got its own challenges.
'I just like winning bike races. The medals are the extra bonus at the end of them.'
In the women's Individual C1-3 race, Zeng Sini of China triumphed in a time of 1:29:02, finishing ahead of Denise Schindler and Allison Jones.
Ukraine's Yegor Dementyev finished 10 seconds ahead of nearest challenger Liu Xinyang in the men's Individual C4-5 race, with Michele Pittacolo back in third.
Dementyev could not contain his excitement afterwards, saying: 'I can't describe this feeling. It is great, wonderful.'
Italian Roberto Bargna claimed gold in the men's C1-3, clocking a winning time of 1:42:51. Steffen Warias and David Nicholas finished second and third respectively.