Disclaimer: I haven't seen multiple sources confirm this (yet). But could Gisele be pissed about her hubby's decision to "un-retire"? Sounds quite plausible IMO.
pagesix.com

Exclusive | Trouble in paradise: Tom Brady and Gisele Bündchen in epic fight
“There’s been trouble in the marriage over his decision to un-retire,” a source told Page Six.

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