Gonzalo Higuain and Ever Banega missed from the spot in a shootout at Estadio Nacional Julio Martinez Pradanos following a drab goalless encounter, as Argentina endured more heartbreak almost a year after losing the World Cup final against Germany.
Higuain blasted high over the crossbar and fellow substitute Banega's tame effort was saved by Claudio Bravo, so Alexis Sanchez had the chance to end Chile's long wait for a Copa title and the Arsenal forward did so in style with a cheeky effort.
Four-time runners-up Chile celebrated in style as Argentina were left to reflect on what might have been once again, as their 22-year wait for a major trophy goes on.
Argentina have now lost two of the last three Copa finals and Lionel Messi - the only Argentina player to score in the shootout - is still to lift a major trophy at international level.
A capacity crowd generated a tremendous atmosphere and Chile, coached by an Argentinian in Jorge Sampaoli, appeared to be inspired as they made an encouraging start.
Eduardo Vargas' long-range strike flashed narrowly wide before Sergio Romero got down to his left to keep out Arturo Vidal's volley following a swift Chile break.
Chile goalkeeper Bravo was then called into action to keep out Sergio Aguero's close-range header after the striker had got on the end of Messi's dangerous free-kick.
The game was being played at a frantic pace and Vargas should have done better when he raced onto a ball over the top of the Argentina defence, but blasted high over the crossbar.
Argentina suffered a blow when Angel di María pulled up with what appeared to be a hamstring injury just before the half-hour mark, with Ezequiel Lavezzi replacing the Manchester United winger - who missed the World Cup final due to a thigh problem.
Lavezzi had a great chance to make an impact when Aguero cut the ball back into his path just before half-time, but the Paris-Saint Germain forward shot straight at Bravo.
Both sides were lacking quality in the final third, but Sanchez almost conjured up a moment of magic to win it when he showed great technique to volley just wide of the far post seven minutes from time.
Argentina had one final chance to snatch victory in normal time when Lavezzi's cross had a little too much on it and Higuain could only fire into the side-netting at full stretch beyond the back post two minutes into time added on.
Sanchez had the only opportunity in the first half of extra time when he raced away following a mistake from Javier Mascherano, but shot just over the crossbar under pressure from the covering Pablo Zabaleta.
Lavezzi appealed for a penalty when he went down under a challenge from Francisco Silva with five minutes remaining, but referee Wilmar Roldan saw nothing untoward and it came as no surprise that the game would be settled by a shootout.
It was advantage Chile when Higuain fired Argentina's second spot-kick high over the bar, then Banega's poor effort was kept out by Bravo to allow Sanchez to win it.
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