The volcano, which unexpectedly burst into life with two eruptions Wednesday evening and Thursday morning, forcing 4,500 people to evacuate, caused alarm again early Friday when it emitted a large puff of smoke.
The head of the National Geology and Mines Service said the volcano was still in "crisis phase," though initial warnings of a possible third eruption have not materialized so far.
The ash cloud meanwhile continued to drift, disrupting flights across a large swath of South America, including one plane from Sydney to Santiago that was forced to turn back after five hours.
Chilean authorities have declared a state of emergency, sent in the army and evacuated a 20-kilometer radius around Calbuco, which is located in Los Lagos, a region popular with tourists for its beautiful mountain landscapes dotted with volcanoes and lakes with black-sand beaches.
Scores of evacuated residents gathered at the police barricade outside the town of La Ensenada, anxious to check on their homes and feed their pets.
On the other side of the security perimeter, the evacuation area was turned into a scattering of ghost towns blanketed with ash up to one meter (three feet) thick, an AFP photographer said.
The weight of the ash caused some roofs to collapse.
Authorities said that if the current conditions held, residents would be allowed to return home for a few hours in the afternoon to retrieve some belongings, after fleeing with nothing but the clothes on their backs.
Ash particles spread over southern Uruguay and a broad belt across central Argentina, though the national weather services said they were at high altitude and did not impair visibility.
"We're still in what is considered the crisis phase," said Rodrigo Alvarez, head of the National Geology and Mines Service. "We cannot rule out a new eruption."
President Michelle Bachelet, who flew to the affected area Thursday, warned the situation remained "unpredictable.
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