By Jonathan Cheng And Ryan Knutson 

Samsung Electronics Co. is leaning on bigger screens and a mobile payment system to try to fend off competition from rivals like Apple Inc. as it battles declining market share in a rapidly slowing smartphone market.

The South Korean company on Thursday unveiled in New York a pair of new devices, including a large-screen variation on its Galaxy S6 Edge flagship handset. So fierce is the competition with Apple that Samsung moved up its event by several weeks to avoid a direct confrontation with Apple, which typically plans a September event to introduce its latest iPhone.

Samsung's Galaxy S6 Edge, first launched in April, was initially a hit with consumers, but the company wasn't able to fully capitalize on the device's popularity due to a misreading of market demand and difficulties in ramping up production of curved screens. Its latest model, known as the Galaxy S6 Edge+, is an effort to regain momentum for its premium smartphones (roughly defined as $450 or more), which drive the bulk of profits in Samsung's mobile division.

Samsung's mobile division has been hit hard as once-explosive growth in the global smartphone market begins to cool. In the second quarter, global smartphone shipments rose 15%, their slowest pace in six years, according to data tracker Strategy Analytics.

Even after the release of the Galaxy S6 Edge earlier this year and its flat-screen counterpart the Galaxy S6, Samsung suffered a 38% drop in operating profit during the second quarter from a year earlier. Its quarterly mobile profits are now less than half what they were just two years ago, at the peak of the company's mobile dominance in 2013.

Compounding the pain, Samsung has lost market share in the wake of last year's release of two hit Apple products, the iPhone 6 and iPhone 6 Plus with its larger screen. Those products cut deeply into Samsung's dominant position in larger-size premium handsets--a corner of the market that it had mostly to itself.

Strategy Analytics said Samsung's market share fell to 21.2% in the second quarter, while Apple, and Chinese competitors like Huawei Technologies Co. and Xiaomi Corp. each gained ground.

On Thursday, Samsung also formally launched its mobile payment service, Samsung Pay, an attempt to compete with Apple, Google Inc. and others on mobile payments. The service is compatible with the three Galaxy S6 smartphones and the new Galaxy Note. It will allow consumers to pay for purchases with their phones at the checkout line.

Like Apple Pay, the Samsung service relies on the traditional payment networks, allowing people to use their existing card accounts. And while Apple's offering only works with next-generation readers, Samsung Pay can be used at checkout counters that use traditional magnetic-strip card readers.

Samsung said the payment service will launch in the U.S. on Sept. 28, after rolling out in Korea on Aug. 20.

Its new mobile offering is an attempt to ride its lead in curved screens during a year when Apple is likely to offer only incremental design changes to its existing iPhone 6 and iPhone 6 Plus devices, said Daniel Gleeson, a senior analyst at IHS Technology.

The Galaxy S6 Edge+ brings the number of Samsung's flagship smartphones this year to three. Samsung also unveiled Thursday the Galaxy Note 5, the fifth iteration in a line of oversize smartphones.

"By bringing out a larger version of the S6 Edge, Samsung is trying to compete with Apple more effectively in that space," Mr. Gleeson said.

On Thursday, Samsung also sought to reposition the Galaxy Note as a productivity-focused device for business consumers. It will offer a detachable hard keyboard, similar to the BlackBerry, once hugely popular among office workers, and it has created a feature called SideSync, which allows consumers to sync messages across phones and computers using Windows or Apple's operating systems. It also teamed up with YouTube to launch a live streaming feature to its camera, called Live Broadcast.

The company teased the coming launch of a smartwatch, called Samsung Gear S2. That device will be unveiled at an event in Berlin on Sept. 3. Both phones will be available in the U.S. and Canada Aug. 21 and online presale begins today at 3 p.m. EDT.

Write to Jonathan Cheng at jonathan.cheng@wsj.com and Ryan Knutson at ryan.knutson@wsj.com

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