Magnificent strikes from Admiral Muskwe and Josh Gordon, on his 23rd birthday, bookended Matthew Wolfe's header in the first half before Muskwe then doubled his tally late on at Oakwell.
City were unchanged from the starting XI which secured a 1-0 victory at Carlisle United in the Checkatrade Trophy last week, although Alex Pascanu and George Thomas returned to the bench.
A frantic start in south Yorkshire allowed Leicester to dominate the early proceedings with wide men Layton Ndukwu and Josh Eppiah asking tough questions of the hosts’ backline.
After just seven minutes, Ndukwu, cutting in from the right, located Sam Hughes in space at the back, but the linesman’s flag was up before his header rebounded off the post.
Later, Tykes shot-stopper Nick Townsend could only watch as Eppiah belted a low drive onto the opposite post, but it deflected back out and the hosts swiftly cleared.
City’s early pressure eventually told on 22 minutes, though, when Muskwe picked his spot with a lovely strike from 18 yards, his second of the new campaign.
The Yorkshiremen levelled the scores seven minutes later as Wolfe nodded Kane Swinburn's cross beyond Max Bramley into the bottom corner.
However, City regained their advantage within 120 seconds. After muscling himself into space in the middle, Gordon launched an audacious 30-yard screamer beyond Townsend.
A largely scrappy second period paid witness to an effective defensive display from Steve Beaglehole's visitors, who limited the Tykes to hopeful efforts from distance.
Substitute Wilberforce Ocran nearly hauled his side level with just over 15 minutes remaining, but his side-footed effort whistled inches wide.
In the end, it was City who found the net once more with Muskwe ghosting into the box and converting from close range with three minutes to go.
A result which further cements his side's impressive start to the new season, Beaglehole will be delighted with the progress being made at Under-23s level.
Hughes was a powerful presence at the back.
While initially procured to operate as a centre back, ex-Chester man Sam Hughes has been utilised in a defensive midfield role in past weeks – with pleasing results.
The 20-year-old returned to his duties at the back in south Yorkshire, alongside Josh Knight, but often advanced forwards to provide support for Hamza Choudhury and Kiernan Dewsbury-Hall.
Gordon Elated With Goal
Foxes forward Josh Gordon spoke to LCFC TV after the Under-23s' victory against Barnsley in the Premier League Cup.
Momentum could have shifted back in Barnsley’s favour after Matthew Wolfe’s excellent header just before the half-four mark.
However, Josh Gordon swung the pendulum back with a sumptuous effort, a strike which typified the turn of skill the former Stafford Rangers man possesses.
Where do we stand?
Muskwe was a threat throughout for City.
The Foxes join Premier League 2 champions Everton on three points on Group F. They are top on goal difference.
Portsmouth and Barnsley, meanwhile, occupy the bottom two places. Once every team has played each other twice, at home and away, the top two advance to the knockout stage.
City return to Premier League 2 duties on Friday with a trip to Hotspur Way to face Tottenham at 1pm before welcoming Swansea City to Holmes Park on Monday 23 October.
Barnsley: Townsend, Wardle, Spratt, Wolfe, Fielding, Lund, Swinburn, Kay, Rowe (Ocran 71), Willard, Williams.
Subs not used: Dolan, Tingle, Miller, Greatorex.
Goal: Wolfe 29.
City: Bramley, Wood, Knight, Hughes, Kaba Sherif, Choudhury (c), Dewsbury-Hall, Muskwe, Ndukwu (Leshabela 76), Gordon (Thomas 45), Eppiah (Pascanu 58).
Subs not used: Yates, Ughelumba, Leshabela.
Goals: Muskwe 22, 87, Gordon 31.
Pictures: Mark Cosgrove
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