By Rita Trichur 

Bank of Montreal, Canada's fourth-largest bank by assets, said it aims to double its customer base in the U.S. to six million people over the next three to five years as it looks to push further into the U.S. retail banking market.

The Toronto-based bank operates as BMO Harris Bank in the U.S., with a presence that is mainly concentrated in the Midwest. BMO Harris Bank currently has about 600 U.S. branches and three million customers and is ranked second largest in Illinois and Wisconsin, as measured by deposits.

Like other Canadian-based lenders, BMO is eyeing expansion in the U.S. as it grapples with slower growth prospects at home. Analysts expect Canadian banks with U.S. operations, such as BMO and Toronto-Dominion Bank, are expected to benefit from an improving U.S. economy this year.

"I don't generally put things out if I don't expect to see it happen within three to five years," Chief Executive Officer Bill Downe said in an interview Tuesday. "I think that's a reasonable time frame," he added.

Part of the bank's growth strategy is, in part, to increase the number of customers in its existing U.S. branches, while keeping a lid on costs. The bank is looking at new technology to help it do that.

Earlier this month, BMO launched the U.S.'s largest cardless ATM network, technology that allows customers to withdraw cash by using their smartphones. The bank said this will speed up transactions and reduce fraud.

Its U.S. launch of Apple Pay, meanwhile, is imminent, said Mr. Downe, referring to technology giant Apple Inc.'s new mobile-payment system.

The bank earlier this month also debuted its first "smart branch," which features video tellers. BMO will open four more of those "smart branches" in the U.S. this year, in a bid to cut down on staffing costs and to extend banking hours. The bank also aims to open new branches in parts of the Chicago metropolitan area where it sees gaps in its footprint.

"You have to remember that BMO Harris Bank was principally a commercial bank until 10 years ago," Mr. Downe said in an interview that followed the bank's annual meeting of shareholders in Toronto. "So, we're building a retail brand."

Write to Rita Trichur at rita.trichur@wsj.com

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