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His reasons were:
Financial
The desire to create a refuge for Catholic settlers.
And it had a milder climate.

Calvert was the proprietor of Avalon, the first sustained English settlement on the island of Newfoundland.

But he was discouraged by the climate and the sufferings of the settlers there, so Calvert looked for a more suitable spot further south and sought a new royal charter to settle the region that was to become the state of Maryland.

Calvert hoped that Maryland would become a safe haven for Catholic settlers from England. It did.

In addition, he was familiar with the fortunes that had been made in tobacco in Virginia, and hoped to recoup some of the financial losses he had sustained in his earlier colonial venture in Newfoundland.

George Calvert died in April 1632, but a charter for "Maryland Colony"
was granted to his son, Cæcilius Calvert, 2nd Lord Baltimore, on June 20, 1632

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